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  • 1.
    Abbas, Ghulam
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Luleå University of Technology, Department of Engineering Sciences and Mathematics, Machine Elements.
    Johansson, Gustav
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Alay-e-Abbas, Syed Muhammad
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Computational Materials Modeling Laboratory, Department of Physics, Government College University, Faisalabad 38040, Pakistan.
    Shi, Yijun
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Machine Elements.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Quasi Three-Dimensional Tetragonal SiC Polymorphs as Efficient Anodes for Sodium-Ion Batteries2023In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 6, no 17, p. 8976-8988Article in journal (Refereed)
    Abstract [en]

    In the present work, we investigate, for the first time, quasi 3D porous tetragonal silicon–carbon polymorphs t(SiC)12 and t(SiC)20 on the basis of first-principles density functional theory calculations. The structural design of these q3-t(SiC)12 and q3-t(SiC)20 polymorphs follows an intuitive rational approach based on armchair nanotubes of a tetragonal SiC monolayer where C–C and Si–Si bonds are arranged in a paired configuration for retaining a 1:1 ratio of the two elements. Our calculations uncover that q3-t(SiC)12 and q3-t(SiC)20 polymorphs are thermally, dynamically, and mechanically stable with this lattice framework. The results demonstrate that the smaller polymorph q3-t(SiC)12 shows a small band gap (∼0.59 eV), while the larger polymorph of q3-t(SiC)20 displays a Dirac nodal line semimetal. Moreover, the 1D channels are favorable for accommodating Na ions with excellent (>300 mAh g–1) reversible theoretical capacities. Thus confirming potential suitability of the two porous polymorphs with an appropriate average voltage and vanishingly small volume change (<6%) as anodes for Na-ion batteries.

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  • 2.
    Busch, Michael
    et al.
    Department of Chemistry, Electrochemistry, University of Gothenburg, S-412 96 Gothenburg, Sweden.
    Ahlberg, E.
    Department of Chemistry, Electrochemistry, University of Gothenburg, S-412 96 Gothenburg, Sweden.
    Panas, I.
    Department of Chemistry and Biotechnology, Energy and Materials, Chalmers University of Technology, S-412 96 Gothenburg, Sweden.
    Electrocatalytic oxygen evolution from water on a Mn(iii–v) dimer model catalyst—A DFT perspective2011In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, no 33, p. 15069-15076Article in journal (Refereed)
  • 3.
    Busch, Michael
    et al.
    Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
    Fabrizio, Alberto
    Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
    Luber, Sandra
    Department of Chemistry and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), University of Zürich, 8057 Zürich, Switzerland.
    Hutter, Jürg
    Department of Chemistry and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), University of Zürich, 8057 Zürich, Switzerland.
    Corminboeuf, Clemence
    Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
    Exploring the Limitation of Molecular Water Oxidation Catalysts2018In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, no 23, p. 12404-12412Article in journal (Refereed)
  • 4.
    Busch, Michael
    et al.
    Department of Chemistry and Material Science, School of Chemical Engineering, Aalto University Kemistintie 1, 02150 Espoo, Finland.
    Laasonen, Kari
    Department of Chemistry and Material Science, School of Chemical Engineering, Aalto University Kemistintie 1, 02150 Espoo, Finland.
    Ahlberg, Elisabet
    Department of Chemistry and Molecular Biology;University of Gothenburg;41296 Gothenburg;Sweden.
    Method for the accurate prediction of electron transfer potentials using an effective absolute potential2020In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 22, no 44, p. 25833-25840Article in journal (Refereed)
  • 5.
    Faisal, Ayad A. H.
    et al.
    Department of Environmental Engineering, College of Engineering, University of Baghdad, Baghdad, Iraq.
    Rashid, Hayder M.
    Department of Environmental Engineering, College of Engineering, University of Baghdad, Baghdad, Iraq.
    Sharma, Gaurav
    College of Materials Science and Engineering, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Research Center for Interfacial Engineering of Functional Materials, Nanshan District Key Lab. for Biopolymers and Safety Evaluation, Shenzhen University, Shenzhen 518055, P.R. China; International Research Centre of Nanotechnology for Himalayan Sustainability (IRCNHS), Shoolini University, Solan 173212, Himachal Pradesh, India; School of Life and Allied Health Sciences, Glocal University, Saharanpur, India.
    Al-Ansari, Nadhir
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Mining and Geotechnical Engineering.
    Saleh, B.
    Mechanical Engineering Department, College of Engineering, Taif University, P.O. Box: 11099, Taif 21944, Saudi Arabia.
    A mathematical model for simulation the removal of cadmium and chromium from groundwater using scrap iron and aluminum as permeable reactive barrier2022In: Desalination and Water Treatment, ISSN 1944-3994, E-ISSN 1944-3986, Vol. 259, p. 186-196Article in journal (Refereed)
    Abstract [en]

    The present work is represented by the derivation of mathematical model and solving the model analytically using the method of separation of variables to describe the migration of the contaminant metal ions through a column packed with bed of permeable reactive barrier (PRB). The validity of the solution can be evaluated through the simulation of cadmium and chromium ions using scrap iron and/or aluminum by-products in the form of wastes that if not utilized to treat waste by waste can impose further burden over the ecosystem. Breakthrough curves proved that the increase of metal ions velocity will decrease the capturing of the ions; therefore, the distribu-tion coefficient and the retardation factor also decrease. Furthermore, the increase of barrier depth will increase the longevity of PRB because this will delay the migration of contaminant. A mathematical model has acceptable ability in the representation of experimental measurements with Nash-€“Sutcliff efficiency coefficients greater than 0.98. The longevity of the PRB was estimated for the field scale to be 210 and 250 d to produce contaminant effluent beyond 100 cm barrier matrix within the environmental permissible concentrations. Although groundwater velocity is highly variable, a proposed velocity of 0.25 cm/min which is assumed to be analogous to the groundwater velocity has revealed prolonged longevity of 7.02 y for the capture of chromium.

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  • 6.
    Khalili, Roya
    et al.
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Kantola, Anu M.
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Komulainen, Sanna
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Selent, Anne
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Selent, Marcin
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland; Centre for Material Analysis, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Vaara, Juha
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Larsson, Anna-Carin
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
    Lantto, Perttu
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    Telkki, Ville-Veikko
    NMR Research Unit, University of Oulu, P.O.Box 3000, FIN-90014, Finland.
    129Xe NMR analysis of pore structures and adsorption phenomena in rare-earth element phosphates2022In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 344, article id 112209Article in journal (Refereed)
    Abstract [en]

    Rare-earth elements (REEs) are indispensable in various applications ranging from catalysis to batteries and they are commonly found from phosphate minerals. Xenon is an excellent exogenous NMR probe for materials because it is inert and its 129Xe chemical shift is very sensitive to its local physical or chemical environment. Here, we exploit, for the first time, 129Xe NMR for the characterization of porous structures and adsorption properties of REE phosphates (REEPO4). We study four different REEPO4 samples (REE = La, Lu, Sm and Yb), including both light (La and Sm) and heavy (Lu and Yb) as well as diamagnetic (La and Lu) and paramagnetic (Sm and Yb) REEs. 129Xe resonances are very sensitive to the porous structures and moisture content of the REEPO4 samples. In the samples treated at a lower temperature (80 °C), free water hinders the access of hydrophobic xenon into small mesopores, but the treatment at a higher temperature (200 °C) removes the free water and allows xenon to explore the mesopores. Based on a standard two-site exchange model analysis of the variable-temperature 129Xe chemical shifts, as well as its proposed, novel modification for paramagnetic materials, the average mesopore sizes were determined. The size was the largest (79 nm) for the La sample with mixed monazite (70%) and rhabdophane (30%) phases and the smallest (6 nm) for the Yb sample with pure xenotime phase. The mesopore sizes of the Lu and Yb samples (12 and 6 nm) differed by a factor of two regardless of their similar xenotime phase. The 129Xe NMR analysis revealed that the heats of adsorption of the samples are similar, varying between 8.7 and 10.1 kJ/mol. For diamagnetic samples, computational modelling confirmed the order of magnitude of the chemical shifts of Xe adsorbed on surfaces and therefore the validity of the two-site exchange model analysis. Overall, 129Xe NMR provides exceptionally versatile information about the pore structures and adsorption properties of REEPO4 materials, which may be very useful for developing the extraction processes and applications of REEs.

  • 7.
    Prajapati, Preeti
    et al.
    Department of Physics, University of Lucknow, Lucknow, India.
    Pandey, Jaya
    Department of Physics, University of Lucknow, Lucknow, India.
    Tandon, Poonam
    Department of Physics, University of Lucknow, Lucknow, India.
    Sinha, Kirti
    Department of Physics, University of Lucknow, Lucknow, India.
    Shimpi, Manishkumar R.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering. Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, Sweden.
    Molecular Structural, Hydrogen Bonding Interactions, and Chemical Reactivity Studies of Ezetimibe-L-Proline Cocrystal Using Spectroscopic and Quantum Chemical Approach2022In: Frontiers in Chemistry, E-ISSN 2296-2646, Vol. 10, article id 848014Article in journal (Refereed)
    Abstract [en]

    Ezetimibe (EZT) being an anticholesterol drug is frequently used for the reduction of elevated blood cholesterol levels. With the purpose of improving the physicochemical properties of EZT, in the present study, cocrystals of ezetimibe with L-proline have been studied. Theoretical geometry optimization of EZT-L-proline cocrystal, energies, and structure–activity relationship was carried out at the DFT level of theory using B3LYP functional complemented by 6-311++G(d,p) basis set. To better understand the role of hydrogen bonding, two different models (EZT + L-proline and EZT + 2L-proline) of EZT-L-proline cocrystal were studied. Spectral techniques (FTIR and FT-Raman) combined with quantum chemical methodologies were successfully implemented for the detailed vibrational assignment of fundamental modes. It is a zwitterionic cocrystal hydrogen bonded with the OH group of EZT and the COO− group of L-proline. The existence and strength of hydrogen bonds were examined by a natural bond orbital analysis (NBO) supported by the quantum theory of atoms in molecule (QTAIM). Chemical reactivity was reflected by the HOMO–LUMO analysis. A smaller energy gap in the cocrystal in comparison to API shows that a cocrystal is softer and chemically more reactive. MEPS and Fukui functions revealed the reactive sites of cocrystals. The calculated binding energy of the cocrystal from counterpoise method was −11.44 kcal/mol (EZT + L-proline) and −26.19 kcal/mol (EZT + 2L-proline). The comparative study between EZT-L-proline and EZT suggest that cocrystals can be better used as an alternative to comprehend the effect of hydrogen bonding in biomolecules and enhance the pharmacological properties of active pharmaceutical ingredients (APIs).

  • 8.
    Szabo, Peter
    et al.
    Department of General and Inorganic Chemistry, Institute of Chemistry, University of Pannonia, P.O.B. 158, Veszprém, H-8201, Hungary.
    Lendvay, György
    Department of General and Inorganic Chemistry, Institute of Chemistry, University of Pannonia, P.O.B. 158, Veszprém, H-8201, Hungary; Institute of Materials and Environmental Chemistry, Research Centre for Natural Sciences, Hungarian Academy of Sciences, Magyar Tudósok krt. 2., Budapest, H-1117, Hungary.
    Dynamics of Complex-Forming Bimolecular Reactions: A Comparative Theoretical Study of the Reactions of H Atoms with O2(3ςg-) and O2(1δg)2015In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 119, no 50, p. 12485-12497Article in journal (Refereed)
  • 9.
    Talwelkar Shimpi, Mayura
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Department of Pharmaceutical Biosciences, Uppsala University, PO Box 591, 75124 Uppsala, Sweden.
    Sajjad, Muhammad
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute, University of Nottingham Ningbo China, Ningbo, People’s Republic of China.
    Öberg, Sven
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Physical binding energies using the electron localization function in 4-hydroxyphenylboronic acid co-crystals with aza donors2023In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648X, Vol. 35, no 50, article id 505901Article in journal (Refereed)
    Abstract [en]

    Binding energies are traditionally simulated using cluster models by computation of each synthon for each individual co-crystal former. However, our investigation of the binding strengths using the electron localization function (ELF) reveals that these can be determined directly from the crystal supercell computations. We propose a new modeling protocol for the computation of physical binding energies directly from bulk simulations using ELF analysis. In this work, we establish a correlation between ELF values and binding energies calculated for co-crystals of 4-hydroxyphenylboronic acid (4HPBA) with four different aza donors using density functional theory with varying descriptions of dispersion. Boronic acids are gaining significant interest in the field of crystal engineering, but theoretical studies on their use in materials are still very limited. Here, we present a systematic investigation of the non-covalent interactions in experimentally realized co-crystals. Prior diffraction studies on these complexes have shown the competitive nature between the boronic acid functional group and the para-substituted phenolic group forming heteromeric interactions with aza donors. We determine the stability of the co-crystals by simulating their lattice energies, and the different dispersion descriptions show similar trends in lattice energies and lattice parameters. Our study bolsters the experimental observation of the boronic acid group as a competitive co-crystal former in addition to the well-studied phenolic group. Further research on correlating ELF values for physical binding could potentially transform this approach to a viable alternative for the computation of binding energies.

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  • 10.
    Talwelkarshimpi, Mayura
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Experimental and Theoretical Studies of Boronic Acids as a Co-Crystal Former2021Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Multi-component molecular crystal materials have become a surging research subject due to their potential for applications in various fields such as pharmaceutics, energetic materials, electronics, etc. Their properties are governed by the arrangement of the constituent molecules and the various non-covalent interactions between them in their solid-state structure. Variation of the constituents based on their interactions can be used to design new materials with tailor made properties in so-called cocrystals, which is a strand of crystal engineering. There is always a demand for new functional groups that can form strong intermolecular interactions such as hydrogen bonds with target molecules in co-crystals, and thus form useful materials. The purpose of this thesis is to explore boronic acids (BA) as a potential co-crystal former in crystal engineering. The inspiration behind the choice of BA was that it can act as a hydrogen bond donor or hydrogen bond acceptor depending upon the complementarity with target molecules and their functional groups. Though BA shows flexibility in adopting different forms, they are not well explored in crystal engineering, especially the number of theoretical studies on BA are very limited.The main objective of this thesis is to gain fundamental understanding of the intermolecular interactions formed by BA such as 4-hydroxyphenylboronic acid (4HPBA) and 4-cyanophenylboronic acid (4CyBA), with traditional hydrogen bond forming potential constituents, of which we have studied 4,4’-bipyridine (bpy), 1,2-bis(4-pyridyl)ethene (bpyee), phenazine (Phen), 1,10-phenanthroline (110Phen), 4,7-phenanthroline (47Phen), and melamine (mel). We have then extended our study by using a bio-active entity, theophylline, as a co-crystal former with various BAs including 4HPBA, 4CyBA, 4-chlorophenylboronic acid (4ClBA), 4-bromophenylboronic acid (4BrBA) and 1,4-phynelendiboronic acid (4BDBA) to improve its stability against humidity. Theophylline is an active pharmaceutical ingredient (API) known for its application in the treatment of acute asthma and in tumor therapy. The solid state structures were determined experimentally using single crystal X-ray diffraction (SXRD). In addition, powder X-ray diffraction (PXRD) and thermogravimetric analysis (TGA) was further used to perform more detailed analyses. These studies were extended by theoretical simulations of intermolecular interaction energies and lattice energies using density functional theory (DFT). The interaction energies were simulated with gas phase simulations using PBE and B3LYP functional using Grimme’s dispersion correction (DFT-D3). While periodic DFT was used to simulate lattice energy and to analyze the interaction energies in detail to establish viable design strategies for new co-crystal materials.Our crystal structure analysis shows that BA prefers to form hydrogen bonds with complementary functional groups rather than interacting with another BA, which can be utilized in design of new multicomponent complexes. This study has also shown that BA competes with phenols, which are well studied in crystal engineering, in forming hydrogen bonds with other co-crystal formers. The interaction energies and electron localization function (ELF) analyses are used to find the strength of the various hydrogen bonds present in the crystal lattice. The lattice energy simulations using periodic DFT has shown the stability of complexes over their single component counterparts. This thesis demonstrates the ability of BA as a potential co-crystal former in the crystal engineering field. It also illustrates that experimental studies along with computational modelling gives good understanding of the structural aspects of a complex which can further be implemented to design new materials.Keywords: crystal engineering, boronic acids, X-ray diffraction, DFT, lattice energies,

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  • 11.
    TalwelkarShimpi, Mayura
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Theoretical investigationof 4-hydroxyphenylboronicacid co-crystals with some aza donors usingdensity functional theorywith dispersion.Manuscript (preprint) (Other (popular science, discussion, etc.))
  • 12.
    Wang, Xiangjian
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Department of Information Engineering, Quzhou College of Technology, Quzhou 324000, China.
    Study of physisorption of aromatic molecules on hydroxylated alpha-SiO2 (001) surface using dispersion-corrected density functional theory2023In: Computational and Theoretical Chemistry, ISSN 2210-271X, E-ISSN 2210-2728, Vol. 1220, article id 113991Article in journal (Refereed)
    Abstract [en]

    In this work, the interactions are investigated in a series of aromatic molecules adsorbed on hydroxylated (0 0 1) surface of α-SiO2 using density functional theory with dispersion correction. It is observed that the van der Waals interactions are strongly dependent on the kind of aromatic molecules. For the molecules of heavy halogen, it shows the strong interaction compared to that of benzene molecule due to its large electron affinity of aromatic molecules. Oxygen-based aromatic molecules are very active and easily to from weak hydrogen bond with hydroxylated surface at tilted configurations. The interaction can be attributed mainly to the weak hydrogen bond and short-range van der Waals interaction. The magnitude of weak hydrogen bond is comparable with that of van der Waals dispersion interaction of benzene ring at flat configuration. For non-polar aromatic molecules, the flat configuration is more stable due to the strong van der Waals interaction of benzene ring. Newly SCAN-rVV10 functional offers precise description for capturing the medium and long-range van der Waals interaction in adsorbate–surface. This study offers theoretical guideline for the design and application of aromatic-based molecules in the fields of catalysis, tribology and electronic devices.

  • 13.
    Zulfiqar, Waqas
    et al.
    Computational Materials Modeling Laboratory, Department of Physics, Government College University, Faisalabad, 38040, Faisalabad, Pakistan.
    Javed, Farrukh
    Computational Materials Modeling Laboratory, Department of Physics, Government College University, Faisalabad, 38040, Faisalabad, Pakistan; Department of Chemical Engineering, McGill University, 845 Sherbrooke St. W, Montreal, Quebec, Canada.
    Abbas, Ghulam
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Alay-e-Abbas, Syed Muhammad
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Computational Materials Modeling Laboratory, Department of Physics, Government College University, Faisalabad, 38040, Faisalabad, Pakistan.
    Stabilizing the dopability of chalcogens in BaZrO3 through TiZr co-doping and its impact on the opto-electronic and photocatalytic properties: A meta-GGA level DFT study2024In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 58, p. 409-415Article in journal (Refereed)
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