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  • 1.
    Ali, Asad
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, ‘‘Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Huang, Guo
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Hussain, Shahid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Luo, Shuiping
    College of Materials Science and Engineering, Shenzhen University, Shenzhen 518060, China.
    Shen, Pei Kang
    School of Resources, Environment and Materials, State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, Nanning, 530004, PR China.
    Zhu, Jinliang
    School of Resources, Environment and Materials, State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, Nanning, 530004, PR China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Emerging strategies and developments in oxygen reduction reaction using high-performance Platinum-based electrocatalysts2023In: Nano Reseach, ISSN 1998-0124, E-ISSN 1998-0000Article, review/survey (Refereed)
  • 2.
    An, Rong
    et al.
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Wu, Muqiu
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
    Zhu, Yudan
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Shah, Faiz Ullah
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Atomic force microscopy probing interactions and microstructures of ionic liquids at solid surfaces2022In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, no 14, p. 11098-11128Article, review/survey (Refereed)
    Abstract [en]

    Ionic liquids (ILs) are room temperature molten salts that possess preeminent physicochemical properties and have shown great potential in many applications. However, the use of ILs in surface-dependent processes, e.g. energy storage, is hindered by the lack of a systematic understanding of the IL interfacial microstructure. ILs on the solid surface display rich ordering, arising from coulombic, van der Waals, solvophobic interactions, etc., all giving near-surface ILs distinct microstructures. Therefore, it is highly important to clarify the interactions of ILs with solid surfaces at the nanoscale to understand the microstructure and mechanism, providing quantitative structure–property relationships. Atomic force microscopy (AFM) opens a surface-sensitive way to probe the interaction force of ILs with solid surfaces in the layers from sub-nanometers to micrometers. Herein, this review showcases the recent progress of AFM in probing interactions and microstructures of ILs at solid interfaces, and the influence of IL characteristics, surface properties and external stimuli is thereafter discussed. Finally, a summary and perspectives are established, in which, the necessities of the quantification of IL–solid interactions at the molecular level, the development of in situ techniques closely coupled with AFM for probing IL–solid interfaces, and the combination of experiments and simulations are argued.

  • 3.
    An, Rong
    et al.
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
    Wu, Nanhua
    Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China.
    Gao, Qingwei
    College of Environmental and Chemical Engineering, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, Shanghai University of Electric Power, Shanghai 200090, China.
    Dong, Yihui
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot, 76100, Israel.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, ‘‘Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Shah, Faiz Ullah
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Fuchs, Harald
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China; Center for Nanotechnology (CeNTech), Westfälische Wilhelms-Universität Münster, 48149 Münster, Germany.
    Integrative Studies of Ionic Liquid Interface Layers: Bridging Experiments, Theoretical Models and Simulations2024In: Nanoscale Horizons, ISSN 2055-6756Article in journal (Refereed)
    Abstract [en]

    Ionic liquids (ILs) are a class of salts existing in the liquid state below 100 C, possessing low volatility, high thermal stability as well as many highly attractive solvent and electrochemical capabilities, etc., making them highly tunable for a great variety of applications, such as lubricants, electrolytes, and soft functional materials. In many applications, ILs are first either physi- or chemisorbed on a solid surface to successively create more functional materials. The functions of ILs at solid surfaces can differ considerably from those of bulk ILs, mainly due to distinct interfacial layers with tunable structures resulting in new ionic liquid interface layer (ILIL) properties and enhanced performance. Due to an almost infinite number of possible combinations among the cations and anions to form ILs, the diversity of various solid surfaces, as well as different external conditions and stimuli, a detailed molecular-level understanding of their structure–property relationship is of utmost significance for a judicious design of IL–solid interfaces with appropriate properties for task-specific applications. Many experimental techniques, such as atomic force microscopy, surface force apparatus, and so on, have been used for studying the ion structuring of ILIL. Molecular Dynamics simulations have been widely used to investigate the microscopic behavior of the ILIL. To interpret and clarify the IL structure and dynamics as well as to predict their properties, it is always beneficial to combine both experiments and simulations as close as possible. In another theoretical model development to bridge the structure and properties of ILIL with performance, thermodynamic (TD) prediction & property modeling has been demonstrated as an effective tool to add the properties and function of the studied nanomaterials. Herein, we present recent findings from applying the multiscale triangle “experiment–molecular simulation–TD modeling” in the studies of ion structuring of ILs in the vicinity of solid surfaces, as well as how it qualitatively and quantitatively correlates to the overall ILs properties, performance, and function. We introduce the most common techniques behind “experiment–molecular simulation–modeling” and how they are applied for studying the ILIL structuring, and we highlight the possibilities of the ILIL structuring in applications such as lubrication and energy storage.

  • 4.
    An, Rong
    et al.
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, China.
    Zheng, Hangbing
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, China.
    Dong, Yihui
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot, Israel.
    Liu, Chang
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Zou, Luyu
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, China.
    Feng, Tao
    Herbert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, China; Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, 41A, Romania; Department of Chemical and Geological Sciences, University of Cagliari, Campus Monserrato ,SS 554 Bivio per Sestu, Monserrato, Italy.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Ti-Si-Zr-Zn Nanometallic Glass Substrate with a Tunable Zinc Composition for Surface-Enhanced Raman Scattering of Cytochrome c2023In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 15, no 21, p. 25275-25284Article in journal (Refereed)
  • 5.
    Barroso da Silva, Fernando L.
    et al.
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Av. café, s/no−campus da USP, BR-14040-903 Ribeirão Preto, SP, Brazil; Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, North Carolina 27695, United States.
    Giron, Carolina Corrêa
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Av. café, s/no−campus da USP, BR-14040-903 Ribeirão Preto, SP, Brazil; Hospital de Clínicas, Universidade Federal do Triângulo Mineiro, Av. Getúlio Guaritá, 38025-440 Uberaba, MG, Brazil.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, P. R. China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania; Department of Chemical and Geological Sciences, Campus Monserrato, University of Cagliari, SS 554 bivio per Sestu, 09042 Monserrato, Italy.
    Electrostatic Features for the Receptor Binding Domain of SARS-COV-2 Wildtype and Its Variants. Compass to the Severity of the Future Variants with the Charge-Rule2022In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 126, no 36, p. 6835-6852Article in journal (Refereed)
    Abstract [en]

    Electrostatic intermolecular interactions are important in many aspects of biology. We have studied the main electrostatic features involved in the interaction of the receptor-binding domain (RBD) of the SARS-CoV-2 spike protein with the human receptor Angiotensin-converting enzyme 2 (ACE2). As the principal computational tool, we have used the FORTE approach, capable to model proton fluctuations and computing free energies for a very large number of protein–protein systems under different physical–chemical conditions, here focusing on the RBD-ACE2 interactions. Both the wild-type and all critical variants are included in this study. From our large ensemble of extensive simulations, we obtain, as a function of pH, the binding affinities, charges of the proteins, their charge regulation capacities, and their dipole moments. In addition, we have calculated the pKas for all ionizable residues and mapped the electrostatic coupling between them. We are able to present a simple predictor for the RBD-ACE2 binding based on the data obtained for Alpha, Beta, Gamma, Delta, and Omicron variants, as a linear correlation between the total charge of the RBD and the corresponding binding affinity. This “RBD charge rule” should work as a quick test of the degree of severity of the coming SARS-CoV-2 variants in the future.

  • 6.
    Corrêa Giron, Carolina
    et al.
    Universidade Federal do Triângulo Mineiro, Departamento de Saúde Coletiva, Rua Vigário Carlos, 38025-350 Uberaba, MG, Brazil. Universidade de São Paulo, Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Av. café, s/no – campus da USP, BR-14040-903 Ribeirão Preto SP, Brazil.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania.
    Barroso da Silva, Fernando L.
    Universidade de São Paulo, Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Av. café, s/no – campus da USP, BR-14040-903 Ribeirão Preto SP, Brazil. Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695, United States.
    On the interactions of the receptor-binding domain of SARS-CoV-1 and SARS-CoV-2 spike proteins with monoclonal antibodies and the receptor ACE22020In: Virus Research, ISSN 0168-1702, E-ISSN 1872-7492, Vol. 285, article id 198021Article in journal (Refereed)
    Abstract [en]

    A new betacoronavirus named SARS-CoV-2 has emerged as a new threat to global health and economy. A promising target for both diagnosis and therapeutics treatments of the new disease named COVID-19 is the coronavirus (CoV) spike (S) glycoprotein. By constant-pH Monte Carlo simulations and the PROCEEDpKa method, we have mapped the electrostatic epitopes for four monoclonal antibodies and the angiotensin-converting enzyme 2 (ACE2) on both SARS-CoV-1 and the new SARS-CoV-2 S receptor binding domain (RBD) proteins. We also calculated free energy of interactions and shown that the S RBD proteins from both SARS viruses binds to ACE2 with similar affinities. However, the affinity between the S RBD protein from the new SARS-CoV-2 and ACE2 is higher than for any studied antibody previously found complexed with SARS-CoV-1. Based on physical chemical analysis and free energies estimates, we can shed some light on the involved molecular recognition processes, their clinical aspects, the implications for drug developments, and suggest structural modifications on the CR3022 antibody that would improve its binding affinities for SARS-CoV-2 and contribute to address the ongoing international health crisis.

  • 7.
    de Villiers Engelbrecht, Leon
    et al.
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Farris, Riccardo
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Vasiliu, Tudor
    Centre of Advanced Research in Bio-nanoconjugates and Biopolymers, Romanian Academy—Petru Poni (PP) Institute of Macromolecular Chemistry, 00487 Iasi, Romania.
    Demurtas, Monica
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Piras, Alessandra
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Cesare Marincola, Flaminia
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Centre of Advanced Research in Bio-nanoconjugates and Biopolymers, Romanian Academy—Petru Poni (PP) Institute of Macromolecular Chemistry, 00487 Iasi, Romania. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University (SU), 106 91 Stockholm, Sweden. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University (NTU), 210009 Nanjing, China.
    Porcedda, Silvia
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Mocci, Francesca
    Dipartimento di Scienze Chimiche e Geologiche, Università degli Studi di Cagliari, S.S. 554 Bivio Sestu, Monserrato, 09042 Cagliari, Italy.
    Theoretical and Experimental Study of the Excess Thermodynamic Properties of Highly Nonideal Liquid Mixtures of Butanol Isomers + DBE2021In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 125, no 2, p. 587-600Article in journal (Refereed)
    Abstract [en]

    Binary alcohol + ether liquid mixtures are of significant importance as potential biofuels or additives for internal combustion engines and attract considerable fundamental interest as model systems containing one strongly H-bonded self-associating component (alcohol) and one that is unable to do so (ether), but that can interact strongly as a H-bond acceptor. In this context, the excess thermodynamic properties of these mixtures, specifically the excess molar enthalpies and volumes (HE and VE), have been extensively measured. Butanol isomer + di-n-butyl ether (DBE) mixtures received significant attention because of interesting differences in their VE, changing from negative (1- and isobutanol) to positive (2- and tert-butanol) with increasing alkyl group branching. With the aim of shedding light on the differences in alcohol self-association and cross-species H-bonding, considered responsible for the observed differences, we studied representative 1- and 2-butanol + DBE mixtures by molecular dynamics simulations and experimental excess property measurements. The simulations reveal marked differences in the self-association of the two isomers and, while supporting the existing interpretations of the HE and VE in a general sense, our results suggest, for the first time, that subtle changes in H-bonded topologies may contribute significantly to the anomalous volumetric properties of these mixtures.

  • 8.
    Dmitriev, Yurij A.
    et al.
    Ioffe Institute, 26 Politekhnicheskaya Street, 194021 St Petersburg, Russia.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, People’s Republic of China. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden.
    Benetis, Nikolas P.
    Department of Chemical Engineering, University of Western Macedonia, Kila Kozani 501 00, Greece.
    H/D isotope effect observed in the isotropic Fermi contact interaction of formyl radical: Experimental and theoretical analysis of the inter- and intra-molecular dynamics2020In: AIP Advances, E-ISSN 2158-3226, Vol. 10, no 12, article id 125309Article in journal (Refereed)
    Abstract [en]

    An unexpected deficit of the computed hyper fine coupling constant in normal formyl HCO radicals, compared to that expected based on the proton to deuteron gyromagnetic ratio of the DCO species, was observed in experimental electron paramagnetic resonance studies of HCO and DCO radicals in a CO solid matrix at cryogenic conditions. Still, the matrix was found to have only a small effect on the anisotropic parts of the magnetic parameter tensors. The underlying isotope effect between the lighter proton and the heavier deuteron on the motional dynamics was verified and elucidated by quantum chemical calculations. The experimental results obtained within a temperature range of 1.4 K–4.2 K require special attention due to the tunneling motions of the molecule and its constituent particles. The effect from vibrational, rotational, and librational motion observed in the molecular states of formyl as a probe, averaged over the dynamics of the low temperature CO matrix isolation, reveals a clear proton isotope effect under both classical and quantum conditions.

  • 9.
    Dong, Yihui
    et al.
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel.
    Gong, Mian
    Herbert Gleiter Institute of Nanoscience, Department of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China.
    Shah, Faiz Ullah
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm SE-10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, ‘‘Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    An, Rong
    Herbert Gleiter Institute of Nanoscience, Department of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Phosphonium-Based Ionic Liquid Significantly Enhances SERS of Cytochrome c on TiO2 Nanotube Arrays2022In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 14, no 23, p. 27456-27465Article in journal (Refereed)
    Abstract [en]

    Surface-enhanced Raman scattering (SERS) is an attractive technique for studying trace detection. It is of utmost importance to further improve the performance and understand the underlying mechanisms. An ionic liquid (IL), the anion of which is derived from biomass, [P6,6,6,14][FuA] was synthesized and used as a trace additive to improve the SERS performance of cytochrome c (Cyt c) on TiO2 nanotube arrays (TNAs). An increased and better enhancement factor (EF) by four to five times as compared to the system without an IL was obtained, which is better than that from using the choline-based amino acid IL previously reported by us. Dissociation of the ILs improved the ionic conductivity of the system, and the long hydrophobic tails of the [P6,6,6,14]+ cation contributed to a strong electrostatic interaction between Cyt c and the TNA surface, thereby enhancing the SERS performance. Atomic force microscopy did verify strong electrostatic interactions between the Cyt c molecules and TNAs after the addition of the IL. This work demonstrates the importance of introducing the phosphonium-based IL to enhance the SERS performance, which will stimulate further development of more effective ILs on SERS detection and other relevant applications in biology.

  • 10.
    Dong, Yihui
    et al.
    Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, CAS, Beijing 100190, China; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China.
    Huo, Feng
    Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, CAS, Beijing 100190, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania.
    Detecting confined fluid behavior by SFA: Past, present, and future2021In: Green Energy & Environment, E-ISSN 2468-0257, Vol. 6, no 2, p. 167-168Article in journal (Refereed)
  • 11.
    Dong, Yihui
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering and Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    State Key Laboratory of Materials-Oriented and Chemical Engineering and Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing, China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden. Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, Iasi, Romania.
    Cao, Wei
    State Key Laboratory of Tribology, Tsinghua University, Beijing, China.
    An, Rong
    Herbert Gleiter Institute of Nanoscience, Nanjing University of Science & Technology, Nanjing, China.
    Lu, Linghong
    State Key Laboratory of Materials-Oriented and Chemical Engineering and Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing, China.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented and Chemical Engineering and Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing, China.
    Determination of the small amount of proteins interacting with TiO2 nanotubes by AFM-measurement2019In: Biomaterials, ISSN 0142-9612, E-ISSN 1878-5905, Vol. 192, p. 368-376Article in journal (Refereed)
    Abstract [en]

    Detecting the small amounts of proteins interacting effectively with the solid film electrodes surface still remains a challenge. To address this, in this work, a new approach was proposed by the combination of the adhesion forces and the molecular interaction measured with AFM. Cytochrome c (Cyt C) interacting effectively with TiO2 nanotube arrays (TNAs) was chosen as a probe. The amounts of Cyt C molecules interacting effectively on TNAs surface (CTNA) range from 5.5×10-12 to 7.0×10-12 mol/cm2 (68.2-86.8 ng/cm2) and they are comparable with the values obtained by the electrochemistry method in the literature, in evidence of the accuracy of this AFM-based approach. The reliability of the proposed approach was further verified by conducting Surface Enhanced Raman Scattering (SERS) measurements and estimating the enhancement factor (EF). This interaction-based AFM approach can be used to accurately obtain the small amounts of adsorbed substances on the solid film electrodes surface in the applications such as biosensors, biocatalysis, and drug delivery, etc.

  • 12.
    Dong, Yihui
    et al.
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P.R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P.R. China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania.
    Cao, Wei
    School of Chemistry, Tel Aviv University, Tel Aviv 69978, Israel.
    He, Hongyan
    CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P.R. China.
    Excellent Protein Immobilization and Stability on Heterogeneous C–TiO2 Hybrid Nanostructures: A Single Protein AFM Study2020In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 36, no 31, p. 9323-9332Article in journal (Refereed)
    Abstract [en]

    Enhancing molecular interaction is critical for improving the immobilization and stability of proteins on TiO2 surfaces. In this work, mesoporous TiO2 materials with varied pore geometries were decorated with phenyl phosphoric acid (PPA), followed by a thermal treatment to obtain chemically heterogeneous C–TiO2 samples without changing the geometry and crystalline structure, which can keep the advantages of both carbon and TiO2. The molecular interaction force between the protein and the surfaces was measured using atomic force microscopy by decomposing from the total adhesion forces, showing that the surface chemistry determines the interaction strength and depends on the amount of partial carbon coverage on the TiO2 surface (∼40–80%). Samples with 58.3% carbon coverage provide the strongest molecular interaction force, consistent with the observation from the detected friction force. Surface-enhanced Raman scattering and electrochemical biosensor measurements for these C–TiO2 materials were further conducted to illustrate their practical implications, implying their promising applications such as in protein detection and biosensing.

  • 13.
    Dong, Yihui
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech University.
    Laaksonen, Aatto
    Department of Materials and Environmental Chemistry Arrhenius Laboratory Stockholm University. Centre of Advanced Research in Bionanoconjugates and Biopolymers Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, Iasi, Romania. State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech University, China.
    Cao, Wei
    State Key Laboratory of Tribology Tsinghua University, Beijing, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech University Nanjing, China.
    AFM Study of pH-Dependent Adhesion of Single Protein to TiO2 Surface2019In: Advanced Materials Interfaces, ISSN 2196-7350, Vol. 6, no 14, article id 1900411Article in journal (Refereed)
    Abstract [en]

    The effect of pH-induced electrostatic conditions on the molecular interaction force of a single lysozyme molecule with TiO2 is investigated using atomic force microscopy (AFM). The force between the charged or neutral lysozyme molecule and the TiO2 surface is measured at different pH from 3.6 to 10.8. It is found to be directly proportional to the contact area, given by an effective diameter of the lysozyme molecule, and is further qualitatively verified by the AFM-measured friction coefficients. The results of the Derjaguin–Landau–Verwey–Overbeek theory show that the pH can change the surface charge densities of both lysozyme and TiO2, but the molecular interaction force at different pH is only dependent on the pH-induced effective diameter of lysozyme. The molecular interaction forces, quantified at the nanoscale, can be directly used to design high-performance liquid chromatography measurements at macroscale by tuning the retention time of a protein under varied pH conditions. They can also be applied to develop a model for predicting and controlling the chromatographic separations of proteins.

  • 14.
    Dong, Yihui
    et al.
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel; State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China; Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, No. 41A, 700487 Iasi, Romania.
    Gao, Qingwei
    State Key Laboratory of Chemical Engineering and School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Molecular Mechanistic Insights into the Ionic-Strength-Controlled Interfacial Behavior of Proteins on a TiO2 Surface2021In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 37, no 39, p. 11499-11507Article in journal (Refereed)
    Abstract [en]

    By adjusting the ionic strengths through changing the concentration of the buffer ions, the molecular force and the interfacial behavior of cytochrome c (Cyt c) and TiO2 are systematically studied. The molecular forces determined by combining the adhesion force and adsorption capacity are found to first increase and then decrease with the increasing ionic strength, with a peak obtained at an ionic strength between 0.8 and 1.0 M. The mechanism is explained based on the dissociation and hydration of ions at the interfaces, where the buffer ions could be completely dissociated at ionic strengths of <0.8 M but were partially associated when the ionic strength increased to a high value (>1.2 M), and the strongest hydration was observed around 1.0 M. The hydrodynamic size and the zeta potential value representing the effective contact area and protein stability of the Cyt c molecule, respectively, are also affected by the hydration and are proportional to the molecular forces. The interfacial behavior of Cyt c molecules on the TiO2 surface, determined through surface-enhanced Raman scattering (SERS), is extremely affected by the ionic strength of the solution as the ion dissociation and hydration also increase the electron transfer ability, where the best SERS enhancement is observed at the ionic strength of around 1.0 M, corresponding to the largest molecular force. Our results provide a detailed understanding at the nanoscale on controlling the protein interfacial behavior with solid surfaces, adjusted by the buffer ions.

  • 15.
    Dong, Yihui
    et al.
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm SE-10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Gong, Mian
    Herbert Gleiter Institute of Nanoscience, Department of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, P.R. China.
    An, Rong
    Herbert Gleiter Institute of Nanoscience, Department of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, P.R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Selective Separation of Highly Similar Proteins on Ionic Liquid-Loaded Mesoporous TiO22022In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 38, no 10, p. 3202-3211Article in journal (Refereed)
    Abstract [en]

    Separating proteins from their mixtures is an important process in a great variety of applications, but it faces difficult challenges as soon as the proteins are simultaneously of similar sizes and carry comparable net charges. To develop both efficient and sustainable strategies for the selective separation of similar proteins and to understand the underlying molecular mechanisms to enable the separation are crucial. In this work, we propose a novel strategy where the cholinium-based amino acid [Cho][Pro] ionic liquid (IL) is used as the trace additive and loaded physically on a mesoporous TiO2 surface for separating two similar proteins (lysozyme and cytochrome c). The observed selective adsorption behavior is explained by the hydration properties of the [Cho][Pro] loaded on the TiO2 surface and their partially dissociated ions under different pH conditions. As the pH is increased from 5.0 to 9.8, the degree of hydration of IL ions also increases, gradually weakening the interaction strength of the proteins with the substrates, more for lysozymes, leading to their effective separation. These findings were further used to guide the detection of the retention behavior of a binary mixture of proteins in high-performance liquid chromatography, where the introduction of ILs did effectively separate the two similar proteins. Our results should further stimulate the use of ILs in the separation of proteins with a high degree of mutual similarity.

  • 16.
    Dong, Yihui
    et al.
    Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm SE-10691, Sweden; State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi 700487, Romania.
    Huo, Feng
    Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.
    Gao, Qingwei
    State Key Laboratory of Chemical Engineering and School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Hydrated Ionic Liquids Boost the Trace Detection Capacity of Proteins on TiO2 Support2021In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 37, no 16, p. 5012-5021Article in journal (Refereed)
    Abstract [en]

    Trace detection based on surface-enhanced Raman scattering (SERS) has attracted considerable attention, and exploiting efficient strategies to stretch the limit of detection and understanding the mechanisms on molecular level are of utmost importance. In this work, we use ionic liquids (ILs) as trace additives in a protein-TiO2 system, allowing us to obtain an exceptionally low limit of detection down to 10–9 M. The enhancement factors (EFs) were determined to 2.30 × 104, 6.17 × 104, and 1.19 × 105, for the three systems: one without ILs, one with ILs in solutions, and one with ILs immobilized on the TiO2 substrate, respectively, corresponding to the molecular forces of 1.65, 1.32, and 1.16 nN quantified by the atomic force microscopy. The dissociation and following hydration of ILs, occurring in the SERS system, weakened the molecular forces but instead improved the electron transfer ability of ILs, which is the major contribution for the observed excellent detection. The weaker diffusion of the hydrated IL ions immobilized on the TiO2 substrate did provide a considerably greater EF value, compared to the ILs in the solution. This work clearly demonstrates the importance of the hydration of ions, causing an improved electron transfer ability of ILs and leading to an exceptional SERS performance in the field of trace detection. Our results should stimulate further development to use ILs in SERS and related applications in bioanalysis, medical diagnosis, and environmental science. 

  • 17.
    Dong, Yihui
    et al.
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel.
    Lin, Weifeng
    Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 76100, Israel.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Arrhenius Laboratory, Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, ‘‘Petru Poni” Institute of Macromolecular Chemistry, 700469 Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Complementary Powerful Techniques for Investigating the Interactions of Proteins with Porous TiO2 and Its Hybrid Materials: A Tutorial Review2022In: Membranes, ISSN 2077-0375, E-ISSN 2077-0375, Vol. 12, no 4, article id 415Article, review/survey (Refereed)
    Abstract [en]

    Understanding the adsorption and interaction between porous materials and protein is of great importance in biomedical and interface sciences. Among the studied porous materials, TiO2 and its hybrid materials, featuring distinct, well-defined pore sizes, structural stability and excellent biocompatibility, are widely used. In this review, the use of four powerful, synergetic and complementary techniques to study protein-TiO2-based porous materials interactions at different scales is summarized, including high-performance liquid chromatography (HPLC), atomic force microscopy (AFM), surface-enhanced Raman scattering (SERS), and Molecular Dynamics (MD) simulations. We expect that this review could be helpful in optimizing the commonly used techniques to characterize the interfacial behavior of protein on porous TiO2 materials in different applications.

  • 18.
    Dong, Yihui
    et al.
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China. Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.
    Wu, Na
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm SE-10691, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, Iasi 700487, Romania.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China.
    Zhang, Suojiang
    Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China.
    Excellent Trace Detection of Proteins on TiO2Nanotube Substrates through Novel Topography Optimization2020In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 124, no 50, p. 27790-27800Article in journal (Refereed)
    Abstract [en]

    For improving the surface-enhanced Raman scattering (SERS) performance of nanomaterials to achieve trace detection of proteins and complex biological systems, structural and topographical control is one of the important strategies. In this work, a facial and effective method to optimize the topography of TiO2 nanotube arrays (TNAs) is demonstrated, together with a significant enhancement of the SERS performance of cytochrome C (Cyt C) on TNAs. An enhancement factor (EF) up to 104, which is obtained with the newly developed method on the basis of the quantification of atomic force microscopy (AFM)-measured interaction force, is achieved, corresponding to a superior detection limit of Cyt C down to 10-7 M. The main reason is that adjusting the fluoride contents in an electrolyte (from 0.4 to 0.1 wt %) can reduce the content and sizes of cracks, as well as the tube ruptures of TNAs, where the fluoride content at 0.2 wt % can successfully provide the excellent and optimized topography of TNAs. The TNAs with the optimized topography, especially those with larger tube diameters, demonstrated the importance of structural integrity on a remarkably excellent SERS performance in the trace detection of proteins. The proposed method will stimulate the development and optimization of the active substrate on the SERS applications in biology, bioanalysis, and nanoscience. © 2020 American Chemical Society.

  • 19.
    Engelbrecht, Leon de Villiers
    et al.
    Department of Chemical and Geological Sciences, University of Cagliari, Cagliari, Italy.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Carbonaro, Carlo Maria
    Department of Physics, University of Cagliari, Cagliari, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Chemical and Geological Sciences, University of Cagliari, Cagliari, Italy; Division of Physical Chemistry, Arrhenius Laboratory, Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Mocci, Francesca
    Department of Chemical and Geological Sciences, University of Cagliari, Cagliari, Italy.
    MD simulations explain the excess molar enthalpies in pseudo-binary mixtures of a choline chloride-based deep eutectic solvent with water or methanol2022In: Frontiers in Chemistry, E-ISSN 2296-2646, Vol. 10, article id 983281Article in journal (Refereed)
    Abstract [en]

    The addition of molecular liquid cosolvents to choline chloride (ChCl)-based deep eutectic solvents (DESs) is increasingly investigated for reducing the inherently high bulk viscosities of the latter, which represent a major obstacle for potential industrial applications. The molar enthalpy of mixing, often referred to as excess molar enthalpy HE—a property reflecting changes in intermolecular interactions upon mixing—of the well-known ChCl/ethylene glycol (1:2 molar ratio) DES mixed with either water or methanol was recently found to be of opposite sign at 308.15 K: Mixing of the DES with water is strongly exothermic, while methanol mixtures are endothermic over the entire mixture composition range. Knowledge of molecular-level liquid structural changes in the DES following cosolvent addition is expected to be important when selecting such “pseudo-binary” mixtures for specific applications, e.g., solvents. With the aim of understanding the reason for the different behavior of selected DES/water or methanol mixtures, we performed classical MD computer simulations to study the changes in intermolecular interactions thought to be responsible for the observed HE sign difference. Excess molar enthalpies computed from our simulations reproduce, for the first time, the experimental sign difference and composition dependence of the property. We performed a structural analysis of simulation configurations, revealing an intriguing difference in the interaction modes of the two cosolvents with the DES chloride anion: water molecules insert between neighboring chloride anions, forming ionic hydrogen-bonded bridges that draw the anions closer, whereas dilution of the DES with methanol results in increased interionic separation. Moreover, the simulated DES/water mixtures were found to contain extended hydrogen-bonded structures containing water-bridged chloride pair arrangements, the presence of which may have important implications for solvent applications.

  • 20.
    Gao, Qingwei
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Wu, Nanhua
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Qin, Yao
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, Iasi, Romania.
    Zhu, Yudan
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Lu, Xiaohua
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Molecular insight into wetting behavior of deep eutectic solvent droplets on ionic substrates: A molecular dynamics study2020In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 319, article id 114298Article in journal (Refereed)
    Abstract [en]

    Wetting behavior of droplets made of choline chloride/urea (1:2), an archetypal deep eutectic solvent mixture, is studied using molecular dynamics simulations. The droplets are placed on a smooth model ionic substrate with positive and negative charges of the same magnitude q (0 e ≤ q ≤ 1.0 e), corresponding to a step-by-step change from a hydrophobic to hydrophilic surface. The molecular microstructure of the droplets and their spatial compositions are systematically studied in details on how they both change while gradually moving from hydrophobic to hydrophilic surface. It is observed that urea initially forms a monolayer on the surface with a planar orientation. This layer slowly shrinks while it becomes laterally more and more constrained. It becomes also molecularly more ordered when the surface becomes hydrophilic, at the same time as the contact angles become larger and larger. The anions (Cl-) are continuously pushed further away from the charged surface. While the contact angle increases and wetting decreases, and urea forms even a secondary stable layer where it changes its orientation and turns to have one of its amines facing up and carbonyl down. The average number of urea-urea H-bonds decreases linearly while the number of ion-pair contacts increases when the urea molecules are separating from the mixture. Our analysis gives a clear molecular understanding of the process and can be useful in many applications from membrane separation to catalysis.

  • 21.
    Gao, Qingwei
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.
    Zhang, Yumeng
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China; Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania.
    Zhu, Yudan
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Zhao, Shuangliang
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China; Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China.
    Chen, Yaojia
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Lu, Xiaohua
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Effect of dimethyl carbonate on the behavior of water confined in carbon nanotube2021In: Chinese Journal of Chemical Engineering, ISSN 1004-9541, E-ISSN 2210-321X, Vol. 31, p. 177-185Article in journal (Refereed)
    Abstract [en]

    The dehydration of water by dimethyl carbonate (DMC) is of great significance for its application in electrochemistry and oil industry. With the rapid development of nanomaterial, one-dimensional (e.g. carbon nanotube (CNT)) and two-dimensional (e.g. lamellar graphene) materials have been widely used for molecular sieving. In this work, the molecular behavior of dimethyl carbonate/water mixture confined in CNT with varying diameters was studied based on molecular dynamics simulation. Due to different van der Waals interactions for the components in the mixtures with the solid surface, DMC molecules are preferentially adsorbed on the inner surface of the pore wall and formed an adsorption layer. Comparing with the pure water molecules confined in CNT, the adsorption DMC layer shows notable effect on the local compositions and microstructures of water molecules under nanoconfinement, which may result in different water mobility. Our analysis shows that the surface-induced DMC molecules can destroy the hydrogen bonding network of water molecules and result in an uniform and dispersed distribution of water molecules in the tube. These clear molecular understandings can be useful in material design for membrane separation.

  • 22.
    Gao, Qingwei
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.
    Zhang, Yumeng
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.
    Xu, Shuting
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.
    Laaksonen, Aatto
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-10691 Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania.
    Zhu, Yudan
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Lu, Xiaohua
    College of Chemical Engineering, State Key Laboratory of Materials-oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, PR China.
    Physicochemical properties and structure of fluid at nano-/micro-interface: Progress in simulation and experimental study2020In: Green Energy & Environment, E-ISSN 2468-0257, Vol. 5, no 3, p. 274-285Article, review/survey (Refereed)
    Abstract [en]

    In modern chemical engineering processes, the involvement of solid/fluid interface is the most important component of process intensification techniques, such as confined membrane separation and catalysis. In the review, we summarized the research progress of the latest theoretical and experimental works to elucidate the contribution of interface to the fluid properties and structures at nano- and micro-scale. We mainly focused on water, alcohol aqueous solution, and ionic liquids, because they are classical systems in interfacial science and/or widely involved in the industrialization process. Surface-induced fluids were observed in all reviewed systems and played a critical role in physicochemical properties and structures of outside fluid. It can even be regarded as a new interface, when the adsorption layer has a strong interaction with the solid surface. Finally, we proposed a perspective on scientific challenges in the modern chemical engineering processes and outlined future prospects.

  • 23.
    Giron, Carolina Corrêa
    et al.
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Ribeirão Preto, SP, Brazil; Universidade Federal do Triângulo Mineiro, Hospital de Clínicas, Uberaba, MG, Brazil.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, PR China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania; Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, Italy.
    Barroso da Silva, Fernando Luís
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Ribeirão Preto, SP, Brazil; Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC, USA.
    Differences between Omicron SARS-CoV-2 RBD and other variants in their ability to interact with cell receptors and monoclonal antibodies2023In: Journal of Biomolecular Structure and Dynamics, ISSN 0739-1102, E-ISSN 1538-0254, Vol. 41, no 12, p. 5707-5727Article in journal (Refereed)
    Abstract [en]

    SARS-CoV-2 remains a health threat with the continuous emergence of new variants. This work aims to expand the knowledge about the SARS-CoV-2 receptor-binding domain (RBD) interactions with cell receptors and monoclonal antibodies (mAbs). By using constant-pH Monte Carlo simulations, the free energy of interactions between the RBD from different variants and several partners (Angiotensin-Converting Enzyme-2 (ACE2) polymorphisms and various mAbs) were predicted. Computed RBD-ACE2-binding affinities were higher for two ACE2 polymorphisms (rs142984500 and rs4646116) typically found in Europeans which indicates a genetic susceptibility. This is amplified for Omicron (BA.1) and its sublineages BA.2 and BA.3. The antibody landscape was computationally investigated with the largest set of mAbs so far in the literature. From the 32 studied binders, groups of mAbs were identified from weak to strong binding affinities (e.g. S2K146). These mAbs with strong binding capacity and especially their combination are amenable to experimentation and clinical trials because of their high predicted binding affinities and possible neutralization potential for current known virus mutations and a universal coronavirus.

  • 24.
    Giron, Carolina Corrêa
    et al.
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Ribeirão Preto, Brazil; Hospital de Clínicas, Universidade Federal do Triângulo Mineiro, Uberaba, Brazil.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Arrhenius Laboratory, Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania.
    Barroso da Silva, Fernando Luís
    Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Universidade de São Paulo, Ribeirão Preto, Brazil; Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC, United States.
    Up State of the SARS-COV-2 Spike Homotrimer Favors an Increased Virulence for New Variants2021In: Frontiers in Medical Technology, E-ISSN 2673-3129, Vol. 3, article id 694347Article in journal (Refereed)
    Abstract [en]

    The COVID-19 pandemic has spread worldwide. However, as soon as the first vaccines—the only scientifically verified and efficient therapeutic option thus far—were released, mutations combined into variants of SARS-CoV-2 that are more transmissible and virulent emerged, raising doubts about their efficiency. This study aims to explain possible molecular mechanisms responsible for the increased transmissibility and the increased rate of hospitalizations related to the new variants. A combination of theoretical methods was employed. Constant-pH Monte Carlo simulations were carried out to quantify the stability of several spike trimeric structures at different conformational states and the free energy of interactions between the receptor-binding domain (RBD) and angiotensin-converting enzyme II (ACE2) for the most worrying variants. Electrostatic epitopes were mapped using the PROCEEDpKa method. These analyses showed that the increased virulence is more likely to be due to the improved stability to the S trimer in the opened state, in which the virus can interact with the cellular receptor, ACE2, rather than due to alterations in the complexation RBD-ACE2, since the difference observed in the free energy values was small (although more attractive in general). Conversely, the South African/Beta variant (B.1.351), compared with the SARS-CoV-2 wild type (wt), is much more stable in the opened state with one or two RBDs in the up position than in the closed state with three RBDs in the down position favoring the infection. Such results contribute to understanding the natural history of disease and indicate possible strategies for developing new therapeutic molecules and adjusting the vaccine doses for higher B-cell antibody production.

  • 25.
    Golets, M.
    et al.
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University.
    Shimpi, Manishkumar
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Wang, Y-L
    Applied Physical Chemistry, Department of Chemistry, KTH Royal Institute of Technology.
    Antzutkin, Oleg
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Glavatskih, Sergei
    System and Component Design, KTH, Royal Institute of Technology , Machine Design, KTH Royal Institute of Technology, SE-10044 Stockholm, Sweden, Department of Physics, Warwick University, Coventry.
    Laaksonen, Aatto
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University.
    Understanding the thermal decomposition mechanism of a halogen-free chelated orthoborate-based ionic liquid: a combined computational and experimental study2016In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, p. 22458-22466Article in journal (Refereed)
    Abstract [en]

    In the last few decades, ionic liquids (ILs) have gained significant attention as lubricants and lubricant additives due to their polar nature, low vapour pressure and tunable physicochemical properties. In this work, quantum chemistry calculations and atomistic Molecular Dynamics (MD) simulations were employed to predict thermal degradation mechanisms of a potential lubricating agent - the tributyloctylphosphonium bis(oxalato)borate ([P4,4,4,8][BOB]) IL. It was found that the onset of decomposition of the studied IL coincides with a cleavage of the B-O bonds in the [BOB](-) anion. Consequently, a series of chemical reactions of the [P4,4,4,8](+) cation with the [BOB](-) anion was triggered yielding alkylboranes, alkenes, trialkylphosphines, CO and CO2. Another ionic system, consisting of [P4,4,4,8][Cl], was also tested for a comparison. Thermogravimetric measurements have shown a higher thermal stability of [P4,4,4,8][BOB] compared to that of [P4,4,4,8][Cl] at least at the initial stage of decomposition, in accord with the presented calculations. Quantum chemical frequency calculations also agreed with the experimental Fourier Transform Infrared (FTIR) spectroscopy results.

  • 26.
    Jiang, Guancong
    et al.
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Cai, Liangcheng
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Wang, Shibo
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania .
    Feng, Xin
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Mu, Liwen
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Zhu, Jiahua
    State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 210009, China.
    Critical Role of Carbonized Cellulose in the Evolution of Highly Porous Biocarbon: Seeing the Structural and Compositional Changes of Spent Mushroom Substrate by Deconvoluted Thermogravimetric Analysis2020In: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 59, no 52, p. 22541-22548Article in journal (Refereed)
    Abstract [en]

    Structural optimization of activated carbon (AC) mainly relies on experience, which depends on the intrinsic structure of biochar, processing conditions, and the interplay of both parties. A fundamental understanding of the pore structure evolution related to the intrinsic structure and composition remains a challenge. In this work, spent mushroom substrate, a rapidly growing byproduct of the mushroom cultivation industry, is used as model biomass to prepare AC under CO2 activation. The structure and composition of the AC products with different activation durations were systematically analyzed with several characterization techniques including N2 adsorption–desorption, scanning electron microscopy, X-ray diffraction, and Raman spectroscopy. A multipeak separation method is developed that enables quantitative analysis of carbonized lignin and carbonized cellulose. A peak area ratio parameter is proposed to describe the retention of cellulose. It is revealed that higher retention of carbonized cellulose corresponds to a larger Brunauer–Emmett–Teller (BET) surface area, demonstrating the dominant role of cellulose in the pore structure development process. This work not only provides a qualitative correlation between cellulose and rich porous structure but also offers a new quantitative tool to understand the structure–composition relationship during the pore evolution process.

  • 27.
    Laaksonen, Aatto
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, People’s Republic of China; Department of Chemical and Geological Sciences, University of Cagliari, Campus Monserrato, Monserrato, Italy.
    Mocci, Francesca
    University of Cagliari, Department of Chemical and Geological Sciences, Campus Monserrato, Monserrato, Italy.
    Section Introduction: Molecular Dynamics Simulations and Reaction Rates2024In: Comprehensive Computational Chemistry / [ed] Manuel Yáñez; Russell J. Boyd, Elsevier , 2024, 1, p. 315-328Chapter in book (Other academic)
  • 28.
    Lengvinaitė, Dovilė
    et al.
    Institute of Chemical Physics, Faculty of Physics, Vilnius University, Vilnius LT-10257, Lithuania.
    Kvedaraviciute, Sonata
    DTU Chemistry, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.
    Bielskutė, Stasė
    Institute of Chemical Physics, Faculty of Physics, Vilnius University, Vilnius LT-10257, Lithuania.
    Klimavicius, Vytautas
    Institute of Chemical Physics, Faculty of Physics, Vilnius University, Vilnius LT-10257, Lithuania.
    Balevicius, Vytautas
    Institute of Chemical Physics, Faculty of Physics, Vilnius University, Vilnius LT-10257, Lithuania.
    Mocci, Francesca
    Università di Cagliari, Dipartimento di Scienze Chimiche e Geologiche, Cittadella Universitaria di Monserrato, Cagliari I-09042, Monserrato, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm 10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Aidas, Kęstutis
    Institute of Chemical Physics, Faculty of Physics, Vilnius University, Vilnius LT-10257, Lithuania.
    Structural Features of the [C4mim][Cl] Ionic Liquid and Its Mixtures with Water: Insight from a 1H NMR Experimental and QM/MD Study2021In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 125, no 48, p. 13255-13266Article in journal (Refereed)
    Abstract [en]

    The 1H NMR chemical shift of water exhibits non-monotonic dependence on the composition of an aqueous mixture of 1-butyl-3-methylimidazolium chloride, [C4mim][Cl], ionic liquid (IL). A clear minimum is observed for the 1H NMR chemical shift at a molar fraction of the IL of 0.34. To scrutinize the molecular mechanism behind this phenomenon, extensive classical molecular dynamics simulations of [C4mim][Cl] IL and its mixtures with water were carried out. A combined quantum mechanics/molecular mechanics approach based on the density functional theory was applied to predict the NMR chemical shifts. The proliferation of strongly hydrogen-bonded complexes between chloride anions and water molecules is found to be the reason behind the increasing 1H NMR chemical shift of water when its molar fraction in the mixture is low and decreasing. The model shows that the chemical shift of water molecules that are trapped in the IL matrix without direct hydrogen bonding to the anions is considerably smaller than the 1H NMR chemical shift predicted for the neat water. The structural features of neat IL and its mixtures with water have also been analyzed in relation to their NMR properties. The 1H NMR spectrum of neat [C4mim][Cl] was predicted and found to be in very reasonable agreement with the experimental data. Finally, the experimentally observed strong dependence of the chemical shift of the proton at position 2 in the imidazolium ring on the composition of the mixture was rationalized. 

  • 29.
    Li, Fangfang
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm 10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Zhang, Xiangping
    CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China; School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Rotten Eggs Revaluated: Ionic Liquids and Deep Eutectic Solvents for Removal and Utilization of Hydrogen Sulfide2022In: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 61, no 7, p. 2643-2671Article, review/survey (Refereed)
    Abstract [en]

    Hydrogen sulfide (H2S) is highly toxic and one of the problematic impurities in industrial gas streams, calling for H2S removal down to single-digit ppm levels to protect health and environment, and not to harm to the downstream processes. Here, we discuss the recent developments and challenges of current H2S removal technologies. Furthermore, we present a comprehensive review of H2S removal in ionic liquids (ILs), IL-based solvents/adsorbents/membranes, and deep eutectic solvents (DESs) due to their unique advantages. We analyze theoretical studies to better understand the microscopic details behind H2S removal. We discuss new research on IL/DES-based H2S removal processes from an industrial perspective. Finally, we summarize the utilization of H2S in IL/DES-based systems for the recovery of sulfur and hydrogen, and synthesis of value-added chemicals. This review will provide both general and in-depth knowledge of the achievements, difficulties, and research priorities in developing novel ILs/DESs for efficient and sustainable H2S removal and utilization.

  • 30.
    Li, Fangfang
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Mocci, Francesca
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato 09042, Italy.
    Zhang, Xiangping
    CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm 10691, Sweden; Center of Advanced Research in Bionanocojugates and biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ionic liquids for CO2 electrochemical reduction2021In: Chinese Journal of Chemical Engineering, ISSN 1004-9541, E-ISSN 2210-321X, Vol. 31, p. 75-93Article, review/survey (Refereed)
    Abstract [en]

    Electrochemical reduction of CO2 is a novel research field towards a CO2-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energy in value-added chemical and fuels. Ionic liquids (ILs), as medium and catalysts (or supporting part of catalysts) have been given wide attention in the electrochemical CO2 reduction reaction (CO2RR) due to their unique advantages in lowering overpotential and improving the product selectivity, as well as their designable and tunable properties. In this review, we have summarized the recent progress of CO2 electro-reduction in IL-based electrolytes to produce higher-value chemicals. We then have highlighted the unique enhancing effect of ILs on CO2RR as templates, precursors, and surface functional moieties of electrocatalytic materials. Finally, computational chemistry tools utilized to understand how the ILs facilitate the CO2RR or to propose the reaction mechanisms, generated intermediates and products have been discussed.

  • 31.
    Li, Yangshuo
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Li, Fangfang
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, P. R. China; University of Cagliari, Department of Chemical and Geological Sciences, Campus Monserrato, SS 554 bivio per Sestu, Monserrato, Italy.
    Wang, Chuan
    Metallurgy Department, Swerim AB, Luleå, Sweden .
    Cobden, Paul
    Metallurgy Department, Swerim AB, Luleå, Sweden .
    Boden, Per
    SMA Mineral AB, Filipstad, Sweden .
    Liu, Yanrong
    CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
    Zhang, Xiangping
    CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Electrochemical CO2 reduction with ionic liquids: review and evaluation2023In: Industrial Chemistry & Materials, ISSN 2755-2608, Vol. 1, no 3, p. 410-430Article, review/survey (Refereed)
    Abstract [en]

    The increasing CO2 emission, as the chief culprit causing numerous environmental problems, could be addressed by the electrochemical CO2 reduction (CO2R) to the added-value carbon-based chemicals. Ionic liquids (ILs) as electrolytes and co-catalysts have been widely studied to promote CO2R owing to their unique advantages. Among the potential products of CO2R, those only containing one carbon atom, named C1 products, including CO, CH3OH, CH4, and syngas, are easier to achieve than others. In this study, we first summarized the research status on CO2R to these C1 products, and then, the state-of-the-art experimental results were used to evaluate the economic potential and environmental impact. Considering the rapid development in CO2R, future scenarios with better CO2R performances were reasonably assumed to predict the future business for each product. Among the studied C1 products, the research focuses on CO, where satisfactory results have been achieved. The evaluation shows that producing CO via CO2R is the only profitable route at present. CH3OH and syngas of H2/CO (1 : 1) as the targeted products can become profitable in the foreseen future. In addition, the life cycle assessment (LCA) was used to evaluate the environmental impact, showing that CO2R to CH4 is the most environmentally friendly pathway, followed by the syngas of H2/CO (2 : 1) and CO, and the further improvement of the CO2R performance can make all the studied C1 products more environmentally friendly. Overall, CO is the most promising product from both economic and environmental impact aspects.

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  • 32.
    Lyubartsev, Alexander
    et al.
    Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, People’s Republic of China; Department of Chemical and Geological Sciences, University of Cagliari, Campus Monserrato, Monserrato, Italy.
    Hierarchical Multiscale Modeling Through Inverse Problem Solving2024In: Comprehensive Computational Chemistry / [ed] Manuel Yáñez; Russell J. Boyd, Elsevier , 2024, 1, p. 622-635Chapter in book (Other academic)
  • 33.
    Ma, Chunyan
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China.
    Laaksonen, Aatto
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden. Department of Chemistry-Ångström Laboratory, Uppsala University, Uppsala, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, Iasi, Romania.
    Liu, Chang
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Lu, Xiaohua
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, China.
    The peculiar effect of water on ionic liquids and deep eutectic solvents.2018In: Chemical Society Reviews, ISSN 0306-0012, Vol. 47, no 23, p. 8685-8720Article, review/survey (Refereed)
    Abstract [en]

    Ionic liquids (ILs) and deep eutectic solvents (DESs) have been suggested as eco-friendly alternatives to organic solvents. A trace amount of water is often unavoidable as impurity, and water is also added on purpose to reduce their problematically high viscosity and lower their high price. Understanding the distinct effects of water on the properties of ILs/DESs is highly important. In this review, we collect published experimental and theoretical results for IL/DES-H2O systems at varied water concentrations and analyze them. Results from mechanistic studies, thermodynamic modelling and advanced experiments are collected and critically discussed. Six commonly studied IL/DES-H2O systems were selected to map experimental observations onto microscopic results obtained in mechanistic studies. A great variety of distinct contours of the excess properties can be observed over the entire compositional range, indicating that the properties of IL/DES-H2O systems are highly unpredictable. Mechanistic studies clearly demonstrate that the added H2O rapidly changes the heterogeneous 3D structures of pure ILs/DESs, leading to very different properties and behaviour. There are similarities between aqueous electrolytes and IL/DES solutions but the bulky and asymmetric organic cations in ILs/DESs do not conform to the standard salt dissolution and hydration concepts. Thermodynamic modelling previously assumes ILs/DESs to be either a neutral ion-pair or completely dissociated ions, neglecting specific ion hydration effects. A new conceptual framework is suggested for thermodynamic modelling of IL/DES-H2O binary systems to enable new technologies for their practical applications.

  • 34.
    Mocci, Francesca
    et al.
    Department of Chemical and Geological Sciences, University of Cagliari, I-09042 Monserrato, Italy.
    de Villiers Engelbrecht, Leon
    Department of Chemical and Geological Sciences, University of Cagliari, I-09042 Monserrato, Italy.
    Olla, Chiara
    Department of Physics, University of Cagliari, I-09042 Monserrato, Italy.
    Cappai, Antonio
    Department of Physics, University of Cagliari, I-09042 Monserrato, Italy.
    Casula, Maria Francesca
    Department of Mechanical, Chemical and Materials Engineering, University of Cagliari, Via Marengo 2, IT 09123 Cagliari, Italy.
    Melis, Claudio
    Department of Physics, University of Cagliari, I-09042 Monserrato, Italy.
    Stagi, Luigi
    Department of Chemistry and Pharmacy, Laboratory of Materials Science and Nanotechnology, University of Sassari, Via Vienna 2, 07100 Sassari, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Chemical and Geological Sciences, University of Cagliari, I-09042 Monserrato, Italy; Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, PetruPoni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda 41A, 700487 Iasi, Romania.
    Carbonaro, Carlo Maria
    Department of Physics, University of Cagliari, I-09042 Monserrato, Italy.
    Carbon Nanodots from an In Silico Perspective2022In: Chemical Reviews, ISSN 0009-2665, E-ISSN 1520-6890, Vol. 122, no 16, p. 13709-13799Article, review/survey (Refereed)
    Abstract [en]

    Carbon nanodots (CNDs) are the latest and most shining rising stars among photoluminescent (PL) nanomaterials. These carbon-based surface-passivated nanostructures compete with other related PL materials, including traditional semiconductor quantum dots and organic dyes, with a long list of benefits and emerging applications. Advantages of CNDs include tunable inherent optical properties and high photostability, rich possibilities for surface functionalization and doping, dispersibility, low toxicity, and viable synthesis (top-down and bottom-up) from organic materials. CNDs can be applied to biomedicine including imaging and sensing, drug-delivery, photodynamic therapy, photocatalysis but also to energy harvesting in solar cells and as LEDs. More applications are reported continuously, making this already a research field of its own. Understanding of the properties of CNDs requires one to go to the levels of electrons, atoms, molecules, and nanostructures at different scales using modern molecular modeling and to correlate it tightly with experiments. This review highlights different in silico techniques and studies, from quantum chemistry to the mesoscale, with particular reference to carbon nanodots, carbonaceous nanoparticles whose structural and photophysical properties are not fully elucidated. The role of experimental investigation is also presented. Hereby, we hope to encourage the reader to investigate CNDs and to apply virtual chemistry to obtain further insights needed to customize these amazing systems for novel prospective applications.

  • 35.
    Mulliri, Simone
    et al.
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, I-09042, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China; Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, 10691, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, 700487, Romania.
    Spanu, Pietro
    Istituto di Chimica Biomolecolare, ICB-CNR-Trav, La Crucca 3, Sassari, 07100, Italy.
    Farris, Riccardo
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, I-09042, Italy.
    Farci, Matteo
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, I-09042, Italy.
    Mingoia, Francesco
    Istituto per lo Studio dei Materiali Nanostrutturati ISMN-CNR, Via U. La Malfa 153, Palermo, I-90146, Italy.
    Roviello, Giovanni
    Istituto di Biostrutture e Bioimmagini, IBB-CNR, Via Mezzocannone 16, Naples, I-80134, Italy.
    Mocci, Francesca
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, I-09042, Italy; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, 700487, Romania.
    Spectroscopic and In Silico Studies on the Interaction of Substituted Pyrazolo[1,2-a]benzo[1,2,3,4]tetrazine-3-one Derivatives with c-Myc G4-DNA2021In: International Journal of Molecular Sciences, ISSN 1661-6596, E-ISSN 1422-0067, Vol. 22, no 11, article id 6028Article in journal (Refereed)
    Abstract [en]

    Herein we describe a combined experimental and in silico study of the interaction of a series of pyrazolo[1,2-a]benzo[1,2,3,4]tetrazin-3-one derivatives (PBTs) with parallel G-quadruplex (GQ) DNA aimed at correlating their previously reported anticancer activities and the stabilizing effects observed by us on c-myc oncogene promoter GQ structure. Circular dichroism (CD) melting experiments were performed to characterize the effect of the studied PBTs on the GQ thermal stability. CD measurements indicate that two out of the eight compounds under investigation induced a slight stabilizing effect (2–4 °C) on GQ depending on the nature and position of the substituents. Molecular docking results allowed us to verify the modes of interaction of the ligands with the GQ and estimate the binding affinities. The highest binding affinity was observed for ligands with the experimental melting temperatures (Tms). However, both stabilizing and destabilizing ligands showed similar scores, whilst Molecular Dynamics (MD) simulations, performed across a wide range of temperatures on the GQ in water solution, either unliganded or complexed with two model PBT ligands with the opposite effect on the Tms, consistently confirmed their stabilizing or destabilizing ability ascertained by CD. Clues about a relation between the reported anticancer activity of some PBTs and their ability to stabilize the GQ structure of c-myc emerged from our study. Furthermore, Molecular Dynamics simulations at high temperatures are herein proposed for the first time as a means to verify the stabilizing or destabilizing effect of ligands on the GQ, also disclosing predictive potential in GQ-targeting drug discovery. 

  • 36.
    Neamtu, Andrei
    et al.
    Department of Physiology, “Grigore T. Popa” University of Medicine and Pharmacy of Iasi, Str. Universitatii nr. 16, 700051 Iasi, România; TRANSCEND Centre – Regional Institute of Oncology (IRO) Iasi, Str. General Henri Mathias Berthelot, Nr. 2–4 Iași, România.
    Mocci, Francesca
    University of Cagliari, Department of Chemical and Geological Sciences, Campus Monserrato, SS 554 bivio per Sestu, 09042 Monserrato, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Centre of Advanced Research in Bionanoconjugates and Biopolymers, PetruPoni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, 41 A, 700487 Iasi, Romania; University of Cagliari, Department of Chemical and Geological Sciences, Campus Monserrato, SS 554 bivio per Sestu, 09042 Monserrato, Italy; Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 210009, PR China.
    Barroso da Silva, Fernando L.
    Universidade de São Paulo, Departamento de Ciências Biomoleculares, Faculdade de Ciências Farmacêuticas de Ribeirão Preto, Av. café, s/no – campus da USP, BR-14040-903 Ribeirão Preto, SP, Brazil; Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695, USA.
    Towards an optimal monoclonal antibody with higher binding affinity to the receptor-binding domain of SARS-CoV-2 spike proteins from different variants2023In: Colloids and Surfaces B: Biointerfaces, ISSN 0927-7765, E-ISSN 1873-4367, Vol. 221, article id 112986Article in journal (Refereed)
    Abstract [en]

    A highly efficient and robust multiple scales in silico protocol, consisting of atomistic Molecular Dynamics (MD), coarse-grain (CG) MD, and constant-pH CG Monte Carlo (MC), has been developed and used to study the binding affinities of selected antigen-binding fragments of the monoclonal antibody (mAbs) CR3022 and several of its here optimized versions against 11 SARS-CoV-2 variants including the wild type. Totally 235,000 mAbs structures were initially generated using the RosettaAntibodyDesign software, resulting in top 10 scored CR3022-like-RBD complexes with critical mutations and compared to the native one, all having the potential to block virus-host cell interaction. Of these 10 finalists, two candidates were further identified in the CG simulations to be the best against all SARS-CoV-2 variants. Surprisingly, all 10 candidates and the native CR3022 exhibited a higher affinity for the Omicron variant despite its highest number of mutations. The multiscale protocol gives us a powerful rational tool to design efficient mAbs. The electrostatic interactions play a crucial role and appear to be controlling the affinity and complex building. Studied mAbs carrying a more negative total net charge show a higher affinity. Structural determinants could be identified in atomistic simulations and their roles are discussed in detail to further hint at a strategy for designing the best RBD binder. Although the SARS-CoV-2 was specifically targeted in this work, our approach is generally suitable for many diseases and viral and bacterial pathogens, leukemia, cancer, multiple sclerosis, rheumatoid, arthritis, lupus, and more.

  • 37.
    Perepelytsya, Sergiy
    et al.
    Bogolyubov Institute for Theoretical Physics of the National Academy of Sciences of Ukraine, Kyiv 03143, Ukraine; National University of Kyiv-Mohyla Academy, Kyiv 04070, Ukraine.
    Vasiliu, Tudor
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania; The Research Institute of the University of Bucharest (ICUB), 90 Sos. Panduri, 050663 Bucharest, Romania.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania; Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, 210009 Nanjing, PR China; Department of Chemical and Geological Sciences, University of Cagliari, 09042, Monserrato, Italy.
    Engelbrecht, Leon De Villiers
    Department of Chemical and Geological Sciences, University of Cagliari, 09042, Monserrato, Italy.
    Brancato, Giuseppe
    Scuola Normale Superiore and CSGI, Piazza dei Cavalieri 7, I-56126 Pisa, Italy; Istituto Nazionale di Fisica Nucleare (INFN) sezione di Pisa, Largo Bruno Pontecorvo 3, I-56127 Pisa, Italy.
    Mocci, Francesca
    Department of Chemical and Geological Sciences, University of Cagliari, 09042, Monserrato, Italy.
    Conformational flexibility of spermidine3+ interacting with DNA double helix2023In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 389, article id 122828Article in journal (Refereed)
    Abstract [en]

    Natural polyamines play a key role in many biological processes, particularly in the stabilization of DNA double helix structure in the cell nucleus. Among others, the conformational flexibility of polyamines, such as spermidine, is an essential property for the formation of complexes with DNA. Yet, the characterization of the conformational space of polyamines has not been fully elucidated. Using atomistic molecular dynamics (MD) simulations, we present a detailed study of the conformational space of spermidine3+ both in solution and in interaction with DNA. We have identified more than 2000 distinct conformations, which can be grouped into seven modes. Notably, the relative population of these modes is highly affected by the interaction of spermidine3+ with DNA, thus representing a fingerprint of complex formation. In particular, three of the seven dihedral angles of spermidine3+ are predominantly in trans conformation (with or without DNA), while the other four dihedral angles are observed to switch between trans, gauche+ and gauche-. The preference between the latter conformational states was analyzed in terms of the distinct energy contributions composing the potential energy. Overall, our results shed some light on the conformational equilibrium and dynamics of spermidine3+, which in turn is important for understanding the nature of its interaction with DNA.

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  • 38.
    Sarman, Sten
    et al.
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487 Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, 210009, P. R. China; Department of Chemical and Geological Sciences, University of Cagliari, Campus Monserrato, SS 554 Bivio per Sestu, 09042, Monserrato, Italy.
    Diffusion-driven rotation in cholesteric liquid crystals studied using molecular dynamics simulation of a mixture of the Gay-Berne fluid and the Lennard-Jones fluid2023In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 25, no 28, p. 18833-18843Article in journal (Refereed)
    Abstract [en]

    Diffusion-driven rotation in cholesteric liquid crystals has been studied using molecular dynamics simulation. Then a chemical potential gradient parallel to the cholesteric axis induces a torque that rotates the director at a constant rate around this axis, besides driving a mass current. An equimolar mixture of Gay-Berne ellipsoids and Lennard-Jones spheres was used as the molecular model. In order to keep the system homogeneous, the color conductivity algorithm was used to apply a color field instead of a chemical potential gradient to drive a mass current. Then the particles are given a color charge that interacts with a color field in the same way as with an electric field, but these charges do not interact with each other. This algorithm is often used to calculate the mutual diffusion coefficient. In the above liquid crystal model, it was found that the color field induces a torque that rotates the director at a constant rate around the cholesteric axis in addition to driving a mass current. The phenomenon was quantified by calculating the cross-coupling coefficient between the color field and the director angular velocity. The results were cross-checked by using a director rotation algorithm to exert a torque to rotate the director at a constant rate. Besides rotation of the director, this resulted in a mass current parallel to the cholesteric axis. The cross-coupling coefficient between the torque and the mass current was equal to the cross-coupling coefficient between the color field and the director rotation rate within a statistical uncertainty of 10 percent, thus fulfilling the Onsager reciprocity relations. As a further cross-check, these cross-coupling coupling coefficients, the color conductivity, and the twist viscosity were calculated by evaluating the corresponding Green-Kubo relations. Finally, it was noted that the orientation of the cholesteric axis parallel to the color field is the one that minimizes the irreversible energy dissipation rate. This is in accordance with a theorem stating that this quantity is minimal in the linear regime of a nonequilibrium steady state.

  • 39.
    Sarman, Sten
    et al.
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, P. R. China; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea, Grigore Ghica-Voda, 41A 700487 Iasi, Romania.
    Microscopic shear flow simulations of a biaxial smectic A liquid crystal based on the soft ellipsoid string-fluid2021In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 23, no 28, p. 15183-15195Article in journal (Refereed)
    Abstract [en]

    We have studied the behaviour of a biaxial smectic A liquid crystal based on the soft ellipsoid string-fluid in shear flow by molecular dynamics simulation using the SLLOD equation of motion. This is facilitated by the fact that the biaxial symmetry allows linear relations between the pressure and the velocity gradient. This means that linear irreversible thermodynamics can be applied independently of the simulations to obtain the torques determining the orientations of the system and that the predictions of this theory can be cross-checked by the simulations. It turns out that there is a torque turning the smectic layers to the orientation parallel to the vorticity plane if the simulation is started in another orientation. In the orientation parallel to the vorticity plane where the director formed by the long axes of the molecules, nw, is perpendicular to the vorticity plane there is another torque keeping the director formed by the normals of the broadsides of the molecules, nu, parallel to this plane at a constant alignment angle, ψ relative to the streamlines independently of the strain rate. Moreover, this alignment angle seems to be the one where the irreversible energy dissipation rate, , is minimal. This is in agreement with a recently proven theorem according to which is minimal in the linear regime of a nonequilibrium steady state. Finally, we studied the orientation of nu when the smectic layers are parallel to the shear plane. In a simulation this orientation is stabilised by the periodic boundary conditions. Then we found that there was a nonlinear torque turning nu to the orientation perpendicular to the streamlines thus minimising the value of even though this value is larger than the value of ẇ in the orientation parallel to the vorticity plane. This means that is minimized given the external boundary conditions.

  • 40.
    Sarman, Sten
    et al.
    Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, People’s Republic of China; University of Cagliari, Department of Chemical and Geological Sciences, Campus Monserrato, Monserrato, Italy.
    Nonequilibrium Molecular Dynamics Simulation of Liquid Crystals and Variational Principle for Nonequilibrium Steady States2023In: Reference Module in Chemistry, Molecular Sciences and Chemical Engineering, Elsevier , 2023Chapter in book (Other academic)
    Abstract [en]

    The purpose of this article is to review molecular dynamics simulation of transport processes of liquid crystal model systems carried out during the last 30 years. In those processes a thermodynamic force or an external dissipative field drives a thermodynamic flux. Well-known examples are shear-flow and elongational flow, where a velocity gradient gives rise to a shear stress, and heat conduction where a temperature gradient drives a heat flow. In these transport processes it has been found that the director of the liquid crystal orients at a constant angle relative to the external dissipative field: In shear-flow the director orients at a constant angle relative to the streamlines, in elongational flow the director is either parallel or perpendicular to the elongation direction and during heat conduction the director is either parallel or perpendicular to the temperature gradient. The alignment angle has been found to be the one that minimizes the irreversible energy dissipation rate. This is in accordance with a recently proven theorem stating that this quantity is minimal in the linear regime of a non-equilibrium steady state. The most commonly used model system is based on the Gay-Berne fluid which can be regarded as a Lennard-Jones fluid generalized to elliptical molecular cores.

  • 41.
    Shen, Gulou
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Jiangsu Provincial Engineering Laboratory for Advanced Materials of Salt Chemical Industry, Huaiyin Institute of Technology, Huaian.
    Laaksonen, Aatto
    Stockholm University, Arrhenius Laboratory, Department oft Materials & Environmental Chemistry.
    Lu, Xiaohua
    Key Laboratory of Material and Chemical Engineering, Nanjing Tech University, Nanjing .
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Developing Electrolyte Perturbed-Chain Statistical Associating Fluid Theory Density Functional Theory for CO2 Separation by Confined Ionic Liquids2018In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, no 27, p. 15464-15473Article in journal (Refereed)
    Abstract [en]

    The electrolyte perturbed-chain statistical associating fluid theory (ePC-SAFT) classical density functional theory (DFT) was developed to describe the behavior of pure ionic liquid (IL) and CO2/IL mixture confined in nanopores, in which a new ionic functional based on the ionic term from ePC-SAFT was proposed for electrostatic free-energy contribution. The developed model was verified by comparing the model prediction with molecular simulation results for ionic fluids, and the agreement shows that the model is reliable in representing the confined behavior of ionic fluids. The developed model was further used to study the behavior of pure IL and CO2/IL mixture in silica nanopores where the IL ions and CO2 were modeled as chains that consisted of spherical segments with the parameters taken from the bulk ePC-SAFT. The results reveal that the nanoconfinement can lead to an increased CO2 solubility, and the solubility increases with increasing pressure. The averaged density of pure IL and solubility of CO2 are strongly dependent on pore sizes and geometries. In addition, the choice of IL ions is very important for the CO2 solubility. Overall, the modeling results for silica-confined systems are consistent with available molecular simulation and experimental results.

  • 42.
    Shukla, Shashi Kant
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Wang, Yong-Lei
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm 10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, ‘‘Petru Poni” Institute of Macromolecular Chemistry, Iasi 700469, Romania; State Key Laboratory of Materials Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Superior gravimetric CO2 uptake of aqueous deep-eutectic solvent solutions2023In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 59, no 70, p. 10516-10519Article in journal (Refereed)
  • 43.
    Sun, Yunhao
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica Voda 41A, 700487 Iasi, Romania.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    How to Detect Possible Pitfalls in ePC-SAFT Modeling. 2. Extension to Binary Mixtures of 96 Ionic Liquids with CO2, H2S, CO, O2, CH4, N2, and H22020In: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 59, no 49, p. 21579-21591Article in journal (Refereed)
    Abstract [en]

    The occurrence of numerical pitfalls has been pointed out for the models of equation of state, including the statistical associating fluid theory (SAFT)-based. Following our previous work on pure ILs when modeling with ePC-SAFT, this work extended the research to the IL–gas mixtures, in which the associating term was derived for predicting the critical point with PC-SAFT, and a scheme for detecting a pitfall in IL–gas mixtures was developed. Then, the scheme was applied to detect the pitfall occurrence in IL–gas (gas = CO2, H2S, CO, O2, CH4, N2, and H2) systems, which are commonly encountered in developing IL-based CO2 separation technologies. It shows that a pitfall occurs only in [C8mpy][BF4]–gas (CO2, H2S, CO, O2, CH4, N2, and H2) among all ILs considered in the temperature and pressure range of interest.

  • 44.
    Sun, Yunhao
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Zuo, Zhida
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China. Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, 106 91, Stockholm, Sweden. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry Aleea Grigore Ghica-Voda, 41A, 700487, Iasi, Romania.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    How to detect possible pitfalls in ePC-SAFT modelling: Extension to ionic liquids2020In: Fluid Phase Equilibria, ISSN 0378-3812, E-ISSN 1879-0224, Vol. 519, article id 112641Article in journal (Refereed)
    Abstract [en]

    An ion-specific electrolyte perturbed-chain statistical associating fluid theory (ePC-SAFT) has been developed to describe the thermodynamic and transport properties of ionic liquids (ILs) for developing IL-based technologies to separate CO2 from gas mixtures. However, as it has been pointed out previously, SAFT-based models can lead to a pitfall, manifesting as an additional fictitious liquid-liquid critical line connected to an additional mechanically stable critical point when modeling pure substances. In this work, a method for detecting a pitfall in ILs was developed, where an expression with ionic term for calculating the critical point with ePC-SAFT was derived and an algorithm for detecting the additional fictitious phase equilibrium for ILs was proposed. The pitfall occurrence for an extended set ILs taken from our previous work was investigated. It shows that a pitfall occurs only for one single IL among all 96 ILs in the temperature and pressure range of interest. For [C8mpy][BF4], at 290.27–291.78 K, a pitfall may occur at the pressures of interest; at 273.15–290.20 K, it may occur at any given pressure. The ion-specific ePC-SAFT parameters for [C8mpy]+ may therefore need to be modified in the future when more reliable experimental results are available for parameter fitting.

  • 45.
    Vasiliu, Tudor
    et al.
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania .
    Craciun, Bogdan Florin
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania .
    Neamtu, Andrei
    Bioinformatics Laboratory, TRANSCEND IRO, Iaşi 700843, Romania .
    Clima, Lilia
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania .
    Isac, Dragos Lucian
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania .
    Maier, Stelian S.
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania; Polymers Research Center, “Gheorghe Asachi” Technical University of Iasi, Iasi, Romania .
    Pinteala, Mariana
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania .
    Mocci, Francesca
    Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania; Dipartimento di Scienze Chimiche e Geologiche, Università di Cagliari, Monserrato, 09042 Cagliari, Italy .
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni” Institute of Macromolecular Chemistry, Iasi 700487, Romania; Department of Materials and Environmental Chemistry, Division of Physical Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, 210009 Nanjing, PR China .
    In silico study of PEI-PEG-squalene-dsDNA polyplex formation: the delicate role of the PEG length in the binding of PEI to DNA2021In: Biomaterials Science, ISSN 2047-4830, E-ISSN 2047-4849, Vol. 9, no 19, p. 6623-6640Article in journal (Refereed)
    Abstract [en]

    Biocompatible hydrophilic polyethylene glycol (PEG) is widely used in biomedical applications, such as drug or gene delivery, tissue engineering or as an antifouling component in biomedical devices. Experimental studies have shown that the size of PEG can weaken polycation-polyanion interactions, like those between branched polyethyleneimine (b-PEI) and DNA in gene carriers, but details of its cause and underlying interactions on the atomic scale are still not clear. To better understand the interaction mechanisms in the formation of polyplexes between b-PEI-PEG based carriers and DNA, we have used a combination of in silico tools and experiments on three multicomponent systems differing in PEG MW. Using the PEI-PEG-squalene-dsDNA systems of the same size, both in the all-atom MD simulations and in experimental in-gel electrophoresis measurements, we found that the binding between DNA and the vectors is highly influenced by the size of PEG, with the binding efficiency increasing with a shorter PEG length. The mechanism of how PEG interferes with the binding between PEI and DNA is explained using a two-step MD simulation protocol that showed that the DNA-vector interactions are influenced by the PEG length due to the hydrogen bond formation between PEI and PEG. Although computationally demanding we find it important to study molecular systems of the same size both in silico and in a laboratory and to simulate the behaviour of the carrier prior to the addition of bioactive molecules to understand the molecular mechanisms involved in the formation of the polyplex.

  • 46.
    Vasiliu, Tudor
    et al.
    Centre of Advanced Research in Bionanoconjugates and Biopolymers “Petru Poni” Institute of Macromolecular Chemistry, Iasi, Romania.
    Mocci, Francesca
    Dipartimento di Scienze Chimiche e Geologiche, Cagliari University, Cagliari, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Centre of Advanced Research in Bionanoconjugates and Biopolymers “Petru Poni” Institute of Macromolecular Chemistry, Iasi, Romania; Dipartimento di Scienze Chimiche e Geologiche, Cagliari University, Cagliari, Italy; Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, China.
    Engelbrecht, Leon De Villiers
    Dipartimento di Scienze Chimiche e Geologiche, Cagliari University, Cagliari, Italy.
    Perepelytsya, Sergiy
    Bogolyubov Institute for Theoretical Physics of the NAS of Ukraine, Kyiv, Ukraine.
    Caging Polycations: Effect of Increasing Confinement on the Modes of Interaction of Spermidine3+ With DNA Double Helices2022In: Frontiers in Chemistry, E-ISSN 2296-2646, Vol. 10, article id 836994Article in journal (Refereed)
    Abstract [en]

    Polyamines have important roles in the modulation of the cellular function and are ubiquitous in cells. The polyamines putrescine2+, spermidine3+, and spermine4+ represent the most abundant organic counterions of the negatively charged DNA in the cellular nucleus. These polyamines are known to stabilize the DNA structure and, depending on their concentration and additional salt composition, to induce DNA aggregation, which is often referred to as condensation. However, the modes of interactions of these elongated polycations with DNA and how they promote condensation are still not clear. In the present work, atomistic molecular dynamics (MD) computer simulations of two DNA fragments surrounded by spermidine3+ (Spd3+) cations were performed to study the structuring of Spd3+ “caged” between DNA molecules. Microsecond time scale simulations, in which the parallel DNA fragments were constrained at three different separations, but allowed to rotate axially and move naturally, provided information on the conformations and relative orientations of surrounding Spm3+ cations as a function of DNA-DNA separation. Novel geometric criteria allowed for the classification of DNA-Spd3+ interaction modes, with special attention given to Spd3+ conformational changes in the space between the two DNA molecules (caged Spd3+). This work shows how changes in the accessible space, or confinement, around DNA affect DNA-Spd3+ interactions, information fundamental to understanding the interactions between DNA and its counterions in environments where DNA is compacted, e.g. in the cellular nucleus.

  • 47.
    Wang, Honglin
    et al.
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Liu, Yanrong
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China. Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Aleea Grigore Ghica-Voda, 41A, 700487, Iasi, Romania. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, SE-106 91 Stockholm, Sweden.
    Krook-Riekkola, Anna
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Yang, Zhuhong
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Lu, Xiaohua
    State Key Laboratory of Material-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, PR China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Carbon recycling – An immense resource and key to a smart climate engineering: A survey of technologies, cost and impurity impact2020In: Renewable & sustainable energy reviews, ISSN 1364-0321, E-ISSN 1879-0690, Vol. 131, article id 110010Article, review/survey (Refereed)
    Abstract [en]

    In order to meet climate goals, both CO2 capture and storage (CCS) and CO2 capture and utilization (CCU) have been identified as increasingly important technologies for mitigating CO2 emissions that are difficult to avoid. In this work, the CO2 utilization, or more specifically, the CO2 conversion to fuels and urea, considering the large demand for CO2, as well as the CO2 mineralization are surveyed and reviewed. The content of this review includes technologies – all the way from the laboratory studies to the industrial applications – their current status, and future potential. CCS is included for a comparison concerning the costs. Also, aspects as the CO2 impurities and the effect of it as well as various requirements concerning the CO2 impurity are included. Many recent studies show that CCU, especially CO2 conversion to fuels, will play an essential role in mitigating CO2 emissions, while developed methods and technologies are not yet mature. More research work needs to be conducted to improve the process efficiency via developing catalysts and reducing the cost of producing H2 that is used as a reactant for fuel synthesis. Moreover, current literature also shows that impurities will affect the process of both CCS and CCU, while the work of studying their influence, especially on CCU, is still scarce. The cost of CCS has been estimated combined with impurities, while studies on cost estimation for CCU are still limited, and the cost, in general, is relatively high with the currently available technologies.

  • 48.
    Wang, Hui
    et al.
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Zuo, Zhida
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Lu, Linghong
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China; Division of Physical Chemistry, Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm 10691, Sweden; Center of Advanced Research in Bionanoconjugates and Biopolymers, “Petru Poni”Institute of Macromolecular Chemistry, Iasi 700469, Romania.
    Wang, Yonglei
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Lu, Xiaohua
    State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Experimental and theoretical study on ion association in [Hmim][halide] + water/isopropanol mixtures2023In: Fluid Phase Equilibria, ISSN 0378-3812, E-ISSN 1879-0224, Vol. 566, article id 113680Article in journal (Refereed)
    Abstract [en]

    The electrical conductivities of the dilute solutions containing ionic liquids (1-hexyl-3-methylimidazolium chloride [Hmim]Cl, 1-hexyl-3-methylimidazolium bromide [Hmim]Br, and 1-hexyl-3-methylimidazolium iodide [Hmim]I) with water and isopropanol were determined in the temperature ranging from 293.15 to 313.15 K. The liquid densities of all binary mixtures were further determined for model parameterization. In theoretical modeling, the limiting molar conductivities Λ0(T) were first obtained using the Debye-Hückel-Onsager (DHO) equation, and thereafter the ion association constants KA(T) were determined using the Shedlovsky equation. The effects of temperature, dielectric constant, and anion size on the values of Λ0(T) and KA(T) were systematically discussed. The Eyring activation enthalpy of charge transport ∆H* and the Walden values Λ0η for all studied binary mixtures were obtained from the temperature-dependent Λ0(T).

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  • 49.
    Wang, Y.L.
    et al.
    Applied Physical Chemistry, Department of Chemistry, KTH Royal Institute of Technology.
    Sarman, Sten
    Applied Physical Chemistry, Department of Chemistry, KTH Royal Institute of Technology.
    Kloo, Lars
    Applied Physical Chemistry, Department of Chemistry, KTH Royal Institute of Technology.
    Antzutkin, Oleg
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Glavatskih, Sergei
    System and Component Design, Department of Machine Design, KTH Royal Institute of Technology.
    Laaksonen, Aatto
    Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University.
    Solvation structures of water in trihexyltetradecylphosphonium-orthoborate ionic liquids2016In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 145, no 6, article id 064507Article in journal (Refereed)
    Abstract [en]

    Atomistic molecular dynamics simulations have been performed to investigate effective interactions of isolated water molecules dispersed in trihexyltetradecylphosphonium-orthoborate ionic liquids (ILs). The intrinsic free energy changes in solvating one water molecule from gas phase into bulk IL matrices were estimated as a function of temperature, and thereafter, the calculations of potential of mean force between two dispersed water molecules within different IL matrices were performed using umbrella sampling simulations. The systematic analyses of local ionic microstructures, orientational preferences, probability and spatial distributions of dispersed water molecules around neighboring ionic species indicate their preferential coordinations to central polar segments in orthoborate anions. The effective interactions between two dispersed water molecules are partially or totally screened as their separation distance increases due to interference of ionic species in between. These computational results connect microscopic anionic structures with macroscopically and experimentally observed difficulty in completely removing water from synthesized IL samples and suggest that the introduction of hydrophobic groups to central polar segments and the formation of conjugated ionic structures in orthoborate anions can effectively reduce residual water content in the corresponding IL samples

  • 50.
    Wang, Yonglei
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden.
    Ji, Xiaoyan
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science.
    Mocci, Francesca
    Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, Italy.
    Laaksonen, Aatto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Energy Science. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, Stockholm, Sweden; Department of Chemical and Geological Sciences, University of Cagliari, Monserrato, Italy; State Key Laboratory of Materials-Oriented and Chemical Engineering, Nanjing Tech University, Nanjing, P. R. CHINA; Centre of Advanced Research in Bionanoconjugates and Biopolymers, Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania.
    The Development of Hierarchical Ion Models and Multiscale Modeling of Tetraalkylphosphonium and Imidazolium Ionic Liquids2023In: Reference Module in Chemistry, Molecular Sciences and Chemical Engineering, Elsevier , 2023Chapter in book (Other academic)
    Abstract [en]

    Ionic liquid (IL) materials are promising electrolytes with striking physicochemical properties for energy and environmental applications. Heterogeneous structures and transport quantities of ILs are intrinsically intercorrelated and span multiple spatiotemporal scales. Multiscale modeling methodology unifying theoretical calculations, atomistic, and coarse-grained simulations based on successive coarse-graining schemes is an efficient approach to explore complex phase behaviors of these ion-containing materials at extended spatiotemporal scales with a modest computational cost. In this chapter, we will provide several examples concentrated on tetraalkylphosphonium and imidazolium ILs showing how to sketch an effective modeling protocol to obtain force field parameters derived at high-resolution scales being transferred to low-resolution levels in a self-consistent computational scheme using a bottom-up approach bridging different length and time scales. Concluding remarks and an outlook on multiscale strategies in understanding and predictive capabilities of ILs and their mixtures are addressed in the final section to highlight future challenges and opportunities associated with IL materials in multiscale modeling community.

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