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Zaeva, A. S., Ivanov, M. A., Gerasimenko, A. V., Ivanov, A. V. & Antzutkin, O. (2020). Dialkyldithiocarbamate platinum(II) complexes of [Pt(S2CNR2)2] (R = iso-C3H7, iso-C4H9): Preparation, 13C CP-MAS NMR, molecular structure, supramolecular self-assembly and thermal behaviour. Polyhedron, 175, Article ID 114166.
Open this publication in new window or tab >>Dialkyldithiocarbamate platinum(II) complexes of [Pt(S2CNR2)2] (R = iso-C3H7iso-C4H9): Preparation, 13C CP-MAS NMR, molecular structure, supramolecular self-assembly and thermal behaviour
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2020 (English)In: Polyhedron, ISSN 0277-5387, E-ISSN 1873-3719, Vol. 175, article id 114166Article in journal (Refereed) Published
Abstract [en]

Two new dialkyldithiocarbamato platinum(II) complexes of [Pt(S2CNR)2], R = iso-C3H7 (1) and iso-C4H9 (2), have been prepared and characterised using 13C CP-MAS NMR. The crystal and molecular structures of the isolated compounds were established by single-crystal X-ray diffraction. The unit cell of 1 contains four centrosymmetric discrete molecules of [Pt{S2CN(iso-C3H7)2}2], of which the pairs are structurally inequivalent to each other (hereafter denoted as molecules 1a and 1b). At the supramolecular level, due to numerous intermolecular C–H···S hydrogen bonds, the 1a molecules form linear polymeric ribbons, whose interaction with the 1b molecules results in a two-dimensional polymeric network. In the structure of 2, the construction of supramolecular zigzag chains by non-centrosymmetric molecules of [Pt{S2CN(iso-C4H9)2}2] is determined by intermolecular C–H···Pt anagostic interactions. The thermal behaviour of crystalline compounds 1 and 2 was studied by simultaneous thermal analysis (STA), a combination of the TG and DSC techniques, under an argon atmosphere. In both cases, platinum(II) sulphide (PtS) was identified as the main end-product upon thermal decomposition of the complexes at 600 °C.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Platinum(II) N, N-dialkyldithiocarbamates, Intermolecular secondary interactions, Supramolecular self-assembly, Thermal transformation of substances, 13C CP-MAS NMR spectroscopy
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-76495 (URN)10.1016/j.poly.2019.114166 (DOI)2-s2.0-85074296446 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-11-19 (johcin)

Available from: 2019-10-24 Created: 2019-10-24 Last updated: 2019-11-19Bibliographically approved
Filippov, A., Antzutkin, O. & Shah, F. U. (2020). Understanding the Interaction of Boric Acid and CO2 with Ionic Liquids in Aqueous Medium by Multinuclear NMR Spectroscopy. ACS Sustainable Chemistry & Engineering, 8, 552-560
Open this publication in new window or tab >>Understanding the Interaction of Boric Acid and CO2 with Ionic Liquids in Aqueous Medium by Multinuclear NMR Spectroscopy
2020 (English)In: ACS Sustainable Chemistry & Engineering, Vol. 8, p. 552-560Article in journal (Refereed) Epub ahead of print
Abstract [en]

Boric acid is known to enhance the kinetics of CO2 absorption by some active aqueous solutions. However, the mechanism of interaction of boric acid with the CO2 in the presence of active molecules is not yet fully understood. In this work, interaction and dynamics of ions in aqueous solutions of functionalized choline-based ionic liquids [N1,1,5,2OH][Threo] and [N1,1,5,2OH][Tau] in the presence of boric acid and CO2 is thoroughly investigated using multinuclear NMR approach: 13C and 11B NMR spectroscopy, 11B NMR transverse relaxation as well as 1H and 11B NMR diffusometry. 13C and 11B NMR spectroscopy has revealed the formation of borate based complexes as a result of reaction between boric acid and anions of the ILs at ionic liquid/boric acid molar ratios larger than ca. 0.15. The formation of these complexes and their dynamics are further investigated using 11B relaxation, and 1H and 11B pulse-field-gradient (PFG) NMR. A plausible reaction mechanisms of boric acid with the anions of the IL, formation of the borate complexes and dissociation of these complexes facilitated by CO2 molecules are suggested.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2020
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-77093 (URN)10.1021/acssuschemeng.9b06068 (DOI)
Available from: 2019-12-07 Created: 2019-12-07 Last updated: 2020-02-20
Korneeva, E., Smolentsev, A. I., Antzutkin, O. & Ivanov, A. V. (2019). Binding of gold(iii) with silver(i) dipropyldithiocarbamate: supramolecular self-assembly (role of secondary Au…S and Ag…S bonds) and thermal behavior of the ionic-polymer complex ([Au(S2CNPr2)2][AgCl2])n. Russian chemical bulletin, 68(1), 40-47
Open this publication in new window or tab >>Binding of gold(iii) with silver(i) dipropyldithiocarbamate: supramolecular self-assembly (role of secondary Au…S and Ag…S bonds) and thermal behavior of the ionic-polymer complex ([Au(S2CNPr2)2][AgCl2])n
2019 (English)In: Russian chemical bulletin, ISSN 1066-5285, E-ISSN 1573-9171, Vol. 68, no 1, p. 40-47Article in journal (Refereed) Published
Abstract [en]

The double ionic-polymer complex ([Au(S2CNPr2)2][AgCl2])n (1) was prepared as an individual fixation form of gold(III) from NaCl solutions with silver(I) dipropyldithiocarbamate and was characterized by single-crystal X-ray diffraction and 13C magic-angle spinning (MAS) NMR spectroscopy. The structure of 1 comprises two nonequivalent centrosymmetric complex cations [Au(S2CNPr2)2]+ (A and B) and the discrete linear anion [AgCl2]. Gold(III) cations are linked by pairs of unsymmetrical secondary Au…S bonds to form linear supramolecular chains (…A…B…)n. Neighboring cations are additionally linked by [AgCl2] anions via secondary Ag…S and Cl…S bonds, the anions being involved in the overall stabilization of the supramolecular structure. The cation–anion interactions lead to a distortion of the linear configuration of the [AgCl2] anion. The character of thermolysis of 1 accompanied by quantitative regeneration of bound Au and Ag was established by simultaneous thermal analysis.

Place, publisher, year, edition, pages
Springer, 2019
Keywords
dialkyldithiocarbamates, binary complexes, noble metals, gold silver compounds, supramolecular self-assembly, secondary interactions, 13C MAS NMR spectroscopy, thermal behavior
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-73818 (URN)10.1007/s11172-019-2413-7 (DOI)000464854400006 ()2-s2.0-85064434277 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-05-02 (johcin)

Available from: 2019-05-02 Created: 2019-05-02 Last updated: 2019-05-02Bibliographically approved
Kotenkov, S. A., Gnezdilov, O. I., Khaliullina, A. V., Antzutkin, O., Gimatdinov, R. S. & Filippov, A. (2019). Effect of Cholesterol and Curcumin on Ordering of DMPC Bilayers. Applied Magnetic Resonance, 50(1-3), 511-520
Open this publication in new window or tab >>Effect of Cholesterol and Curcumin on Ordering of DMPC Bilayers
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2019 (English)In: Applied Magnetic Resonance, ISSN 0937-9347, E-ISSN 1613-7507, Vol. 50, no 1-3, p. 511-520Article in journal (Refereed) Published
Abstract [en]

In this work, we compared the effects of curcumin and cholesterol directly competing to insert into the DMPC lipid bilayer during bilayer formation from an initially non-ordered state. 2H and 14N nuclear magnetic resonance spectroscopy showed that curcumin is not embedded deep in the lipid bilayer and interacts mainly with the head group of the lipid. In a more complex system of DMPC/CHOL/CUR, curcumin amplifies the effect of cholesterol on the ordering of lipid acyl chains.

Place, publisher, year, edition, pages
Springer, 2019
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-72752 (URN)10.1007/s00723-018-1102-2 (DOI)000458124800036 ()2-s2.0-85057198967 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-03-08 (johcin)

Available from: 2019-01-31 Created: 2019-01-31 Last updated: 2019-03-08Bibliographically approved
Rohlmann, P., Munavirov, B., Furó, I., Antzutkin, O., Rutland, M. W. & Glavatskih, S. (2019). Non-halogenated Ionic Liquid Dramatically Enhances Tribological Performance of Biodegradable Oils. Frontiers in Chemistry, 7, Article ID 98.
Open this publication in new window or tab >>Non-halogenated Ionic Liquid Dramatically Enhances Tribological Performance of Biodegradable Oils
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2019 (English)In: Frontiers in Chemistry, E-ISSN 2296-2646, Vol. 7, article id 98Article in journal (Refereed) Published
Abstract [en]

It is demonstrated that a phosphonium orthoborate ionic liquid may serve as a wear reducing additive in biodegradable oils at steel-steel surfaces in the boundary lubrication regime. Tribological tests were performed in a ball-on-three plate configuration. A set of surface characterization techniques—SEM/EDS, FIB and white light interferometry were used to characterize surfaces following the tribotests and to observe the formation of any tribofilms. 11B NMR was used to follow changes in the composition of the ionic-liquid-oil blends and to identify boron-containing decomposition products after the tribotests. The ionic liquid reduces the wear of steel surfaces by up to 92% compared to the neat oil at 90°C; it is shown that the reduction in wear can be correlated with the formation of boron enriched patches in the boundary films.

Place, publisher, year, edition, pages
Laussanne: Frontiers Media S.A., 2019
Keywords
NMR, biodegradable oil, boundary lubrication, friction, ionic liquid, wear
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-73314 (URN)10.3389/fchem.2019.00098 (DOI)000459858200001 ()30891442 (PubMedID)2-s2.0-85068538860 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-03-26 (oliekm)

Available from: 2019-03-26 Created: 2019-03-26 Last updated: 2019-08-22Bibliographically approved
Novikova, E. V., Ivanov, A. V., Egorova, I. V., Troshina, R. S., Rodionova, N. A., Smolentsev, A. I. & Antzutkin, O. (2019). Principles of the Construction of Polymer Structures, Heteronuclear (13C, 15N) CP-MAS NMR, and Thermal Behavior of Heteroleptic Bismuth(III) Complexes of the General Composition [Bi(S2CNR2)2X] (X = NO3, Cl). Russian journal of coordination chemistry, 45(10), 695-705
Open this publication in new window or tab >>Principles of the Construction of Polymer Structures, Heteronuclear (13C, 15N) CP-MAS NMR, and Thermal Behavior of Heteroleptic Bismuth(III) Complexes of the General Composition [Bi(S2CNR2)2X] (X = NO3, Cl)
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2019 (English)In: Russian journal of coordination chemistry, ISSN 1070-3284, E-ISSN 1608-3318, Vol. 45, no 10, p. 695-705Article in journal (Refereed) Published
Abstract [en]

The crystalline heteroleptic bismuth(III) complexes, [Bi{S2CN(iso-C4H9)2}2(NO3)] (I) and [Bi{S2CN(C3H7)2}2Cl] (II), are isolated in preparative yields. Both compounds form 1D polymer structures and are characterized by X-ray diffraction analysis (CIF files CCDC nos. 1877115 (I) and 1876364 (II)) and (13C, 15N) CP-MAS NMR spectroscopy. The coordination mode of each of the dialkyldithiocarbamate ligands is S,S′-anisobidentately terminal. The inorganic anions performing the μ2-bridging function participate in the binding of the adjacent metallic atoms to form zigzag polymer chains. A new mode of bismuth(III) binding involving all oxygen atoms (O,O'-anisobidentate coordination to each adjacent bismuth atom) is found for the bridging nitrate groups in compound I. The bismuth atoms in the studied compounds are characterized by the eightfold [BiS4O4] (I) or sixfold [BiS4Cl2] (II) environment. The thermal behavior of the synthesized complexes is characterized by the data of simultaneous thermal analysis, using parallel recording of thermogravimetry and differential scanning calorimetry curves. In both cases, Bi2S3 is the only final product of the thermal transformations of compounds I and II.

Place, publisher, year, edition, pages
Springer, 2019
Keywords
heteroleptic bismuth(III) complexes, dialkyldithiocarbamate ligands, 1D polymer structures, thermal behavior, X-ray diffraction analysis, heteronuclear (13C 15N) MAS NMR spectroscopy
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-76432 (URN)10.1134/S1070328419100038 (DOI)000488841700004 ()2-s2.0-85073207914 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-10-18 (johcin)

Available from: 2019-10-18 Created: 2019-10-18 Last updated: 2019-10-21Bibliographically approved
Filippov, A., Antzutkin, O. & Shah, F. U. (2019). Rapid carbene formation increasing ion diffusivity in an imidazolium acetate ionic liquid confined between polar glass plates. Physical Chemistry, Chemical Physics - PCCP, 21(40), 22531-22538
Open this publication in new window or tab >>Rapid carbene formation increasing ion diffusivity in an imidazolium acetate ionic liquid confined between polar glass plates
2019 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 21, no 40, p. 22531-22538Article in journal (Refereed) Published
Abstract [en]

1-Ethyl-3-methyl-imidazolium acetate ([EMIM][OAc]) is one of the most widely used ionic liquids for various applications. This study is focussed on the chemical stability of [EMIM][OAc] on the surfaces of polar glass plates. 1H and 13C NMR spectroscopy and NMR diffusometry of [EMIM][OAc] IL confined between glass plates with a specific surface area 105–106 m−1 are thoroughly investigated. A rapid and spontaneous reaction took place on the surfaces of glass plates leading to the formation of neutral chemical moieties as evident by the appearance of new signals in the 1H NMR spectra. These new products are assigned as N-heterocyclic carbene (NHC) and acetic acid. These neutral chemical moieties have significantly increased the ion diffusivity by dissociation of the cation and the anion in [EMIM][OAc] IL. The yield and rate of formation of NHC and acetic acid are found to increase with the increasing surface area of polar glass plates and the time of contact between the IL and glass surfaces. Based on NMR spectroscopy, a dissociative reaction mechanism is proposed for the formation of free NHC in the neat [EMIM][OAc] IL.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Natural Sciences Chemical Sciences Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-76117 (URN)10.1039/C9CP04504J (DOI)31588443 (PubMedID)2-s2.0-85073483050 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-10-25 (johcin)

Available from: 2019-09-25 Created: 2019-09-25 Last updated: 2019-11-04Bibliographically approved
Filippov, A., Antzutkin, O. & Shah, F. U. (2019). Reactivity of CO2 with aqueous choline-based ionic liquids probed by solid-state NMR spectroscopy. Journal of Molecular Liquids, 286, Article ID 110918.
Open this publication in new window or tab >>Reactivity of CO2 with aqueous choline-based ionic liquids probed by solid-state NMR spectroscopy
2019 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 286, article id 110918Article in journal (Refereed) Published
Abstract [en]

CO2 absorption in a series of choline-based ionic liquids is investigated using solid-state 13C and 15N MAS NMR spectroscopy. Natural abundance and 13C enriched CO2 gas was purged through 50 wt% aqueous solutions of alkyldimethyl(2-hydroxyethyl)ammonium threonine, [N1,1,n,2OH][Threo], (alkyl = butyl, pentyl and hexyl) and pentyldimethyl(2-hydroxyethyl)ammonium taurine [N1,1,5,2OH][Tau]. The process of CO2 absorption results in precipitation of a solid sediment, which stays in equilibrium with the liquid phase. Upon degassing of the sample, the sediment is dissolved back into the IL-aqueous phase. Solid state 13C and 15N MAS NMR data suggest that the solid sediment is composed of neutral threonine (or taurine) in the zwitterionic forms and the liquid phase contained the products of reactions between the ionic liquids and CO2 molecules. A plausible mechanism for formation of the solid sediments and the reaction products in liquid phases is suggested.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
CO2 absorption, Aqueous choline-based ionic liquids, Liquid-solid equilibrium, 13C and 15N MAS, CP-MAS NMR
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-73873 (URN)10.1016/j.molliq.2019.110918 (DOI)000474308400033 ()2-s2.0-85065237523 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-05-14 (johcin)

Available from: 2019-05-07 Created: 2019-05-07 Last updated: 2019-08-16Bibliographically approved
Filippov, A., Gnezdilov, O. I., Luchkin, A. G. & Antzutkin, O. (2019). Self-diffusion of ethylammonium nitrate ionic liquid confined between modified polar glasses. Journal of Molecular Liquids, 284, 366-371
Open this publication in new window or tab >>Self-diffusion of ethylammonium nitrate ionic liquid confined between modified polar glasses
2019 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 284, p. 366-371Article in journal (Refereed) Published
Abstract [en]

Ethylammonium nitrate (EAN) ionic liquid confined between flat polar glass platesdemonstrates variable diffusivity that is sensitive to an external static magnetic field. Outside the magnetic field, diffusivity between the plates is higher than that in the bulk. However, after placing the system in a strong static magnetic field, the diffusivity gradually decreased. These processes occur during transformations between phases formed in EAN subjected to micrometer-size restrictions outside and within the magnetic field (Filippov et al., JMolLiq. [2018] 268, 49). In this study, we used samples of two types: (i) with roughened surface formed by treatment of the glass plates with aqueous solutions of hydrofluoric acid and (ii) with vacuum deposited TiO2 layers with a thickness of ca. 1 μm at glass-plate edges. Neither the surface modification of the glass plates, nor the TiO2 layers controlled thickness of EAN confined between glass-plates significantly changed the above-described effects, which have been observed in studies using untreated glass plates. Therefore, the range of systems with detected phase transformations in EAN and accompanying effects, such as accelerated diffusivity and change in diffusivity under the influence of a static magnetic field, was expanded to the systems with roughened surfaces and the systems with TiO2 layers controlled inter-plates distances. Results of experiments with roughened surfaces additionally suggested that the phase transformation of confined EAN in the external magnetic field is isotropic in nature rather than a phase transition from “layered to bulk” structures.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Nuclear magnetic resonance, DiffusivityIon dynamics, Phase transformations, Restricted diffusion
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-73599 (URN)10.1016/j.molliq.2019.04.021 (DOI)000469154300043 ()2-s2.0-85064072853 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-04-11 (johcin)

Available from: 2019-04-11 Created: 2019-04-11 Last updated: 2019-06-19Bibliographically approved
Loseva, O., Rodina, T., Ivanov, A., Smolentsev, A. & Antzutkin, O. (2019). Tetranuclear heteroleptic mercury(ii) complexes of the composition [Hg4(S2CNPr2)6(NO3)2] and [Hg4(S2CNPr2)4Cl4]: structural organization, principles of construction of supramolecular polymeric chains, and thermal behavior. Russian chemical bulletin, 68(4), 782-792
Open this publication in new window or tab >>Tetranuclear heteroleptic mercury(ii) complexes of the composition [Hg4(S2CNPr2)6(NO3)2] and [Hg4(S2CNPr2)4Cl4]: structural organization, principles of construction of supramolecular polymeric chains, and thermal behavior
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2019 (English)In: Russian chemical bulletin, ISSN 1066-5285, E-ISSN 1573-9171, Vol. 68, no 4, p. 782-792Article in journal (Refereed) Published
Abstract [en]

New heteroleptic mercury(ii) complexes [Hg4(S2CNPr2)6(NO3)2] (1) and [Hg4(S2CNPr2)4Cl4] (2) were synthesized and characterized by single-crystal X-ray dif raction and 13C and 15N MAS NMR spectroscopy. In these complexes, the metal atoms are linked in pairs by bridging dipropyldithiocarbamate ligands (Pr2Dtc) to form tetranuclear cations and molecules. The further structural organization of compound 1 to the polymeric chains [Hg4(S2CNPr2)6(NO3)2]n occurs due to the linking of [Hg4(S2CNPr2)6]2+ cations by pairs of bridging nitrate groups. The formation of the supramolecular polymeric structure of 2 is determined by pairwise secondary Hg⋯Cl bonds between the cyclic [Hg4(S2CNPr2)4Cl4] molecules, in which the central eight-membered metallocycle [Hg4S4] adopts a distorted chair conformation. The thermal behavior of compounds 1 and 2 was studied by simultaneous thermal analysis.

Place, publisher, year, edition, pages
Springer, 2019
Keywords
tetranuclear mercury(ii) complexes, polymeric compounds, dialkyldithiocarbamates, supramolecular self-organization, secondary interactions, thermal behavior
National Category
Physical Chemistry
Research subject
Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-74687 (URN)10.1007/s11172-019-2486-3 (DOI)000468612300015 ()2-s2.0-85066120856 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-06-18 (johcin)

Available from: 2019-06-18 Created: 2019-06-18 Last updated: 2019-06-18Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-1067-7990

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