Voronoi Polyhedra as a Tool for the Characterization of Inhomogeneous Distribution in 1-Butyl-3-methylimidazolium Cation-Based Ionic Liquids
- Volodymyr KovergaVolodymyr KovergaLaboratoire de Spectrochimie Infrarouge et Raman, UMR CNRS A8516, Université de Lille, Science et Technologies, 59655 Villeneuve d’Ascq Cedex, FranceInstitut des Sciences Analytiques et de Physico-Chimie pour l’Environnement et les Matériaux (IPREM), Université de Pau et des Pays de l’Adour, Technopôle Helioparc, 2, Avenue Pierre Angot, 64053 Pau Cedex 9, Nouvelle Aquitaine, FranceMore by Volodymyr Koverga
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- Nishith MaityNishith MaityLaboratoire de Spectrochimie Infrarouge et Raman, UMR CNRS A8516, Université de Lille, Science et Technologies, 59655 Villeneuve d’Ascq Cedex, FranceMore by Nishith Maity
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- François Alexandre MiannayFrançois Alexandre MiannayLaboratoire de Spectrochimie Infrarouge et Raman, UMR CNRS A8516, Université de Lille, Science et Technologies, 59655 Villeneuve d’Ascq Cedex, FranceMore by François Alexandre Miannay
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- Oleg N. KaluginOleg N. KaluginDepartment of Inorganic Chemistry, V.N. Karazin Kharkiv National University, Svoboda Square 4, Kharkiv 61022, UkraineMore by Oleg N. Kalugin
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- Akos JuhaszAkos JuhaszLaboratory of Nanochemistry, Department of Biophysics Radiation Biology, Semmelweis University, Nagyvárad tér 4, Budapest 1089, HungaryMore by Akos Juhasz
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- Adam ŚwiątekAdam ŚwiątekLaboratory of Spectroscopy and Intermolecular Interactions, Department of Chemistry, University of Warsaw, ul. Żwirki i Wigury 101, 02-089 Warsaw, PolandMore by Adam Świątek
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- Kamil PolokKamil PolokLaboratory of Spectroscopy and Intermolecular Interactions, Department of Chemistry, University of Warsaw, ul. Żwirki i Wigury 101, 02-089 Warsaw, PolandMore by Kamil Polok
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- Toshiyuki TakamukuToshiyuki TakamukuDepartment of Chemistry and Applied Chemistry, Faculty of Science and Engineering, Saga University, Honjo-machi, Saga 840-8502, JapanMore by Toshiyuki Takamuku
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- Pál Jedlovszky*Pál Jedlovszky*Email: [email protected]Department of Chemistry, Eszterházy Károly University, Leányka utca 6, H-3300 Eger, HungaryMore by Pál Jedlovszky
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- Abdenacer Idrissi*Abdenacer Idrissi*Email: [email protected]Laboratoire de Spectrochimie Infrarouge et Raman, UMR CNRS A8516, Université de Lille, Science et Technologies, 59655 Villeneuve d’Ascq Cedex, FranceMore by Abdenacer Idrissi
Abstract
The inhomogeneity distribution in four imidazolium-based ionic liquids (ILs) containing the 1-butyl-3-methylimidazolium (C4mim) cation, coupled with tetrafluoroborate (BF4), hexafluorophosphate (PF6), bis(trifluoromethanesulfonyl)amide (TFSA), and trifluoromethanesulfonate (TfO) anions, was characterized using Voronoi polyhedra. For this purpose, molecular dynamic simulations have been performed on the isothermal–isobaric (NpT) ensemble. We checked the ability of the potential models to reproduce the experimental density, heat of vaporization, and transport properties (diffusion and viscosity) of these ionic liquids. The inhomogeneity distribution of ions around the ring, methyl, and butyl chain terminal hydrogen atoms of the C4mim cation was investigated by means of Voronoi polyhedra analysis. For this purpose, the position of the C4mim cation was described successively by the ring, methyl, and butyl chain terminal hydrogen atoms, while that of the anions was described by their F or O atom. We calculated the Voronoi polyhedra distributions of the volume, the density, and the asphericity parameters as well as that of the radius of the spherical intermolecular voids. We carried out the analysis in two steps. In the first step, both ions were taken into account. The calculated distributions gave information on the neighboring ions around a reference one. In the second step, to distinguish between like and oppositely charged ions and then to get information on the inhomogeneity distribution of the like ions, we repeated the same calculations on the same sample configurations and removed one of the ions and considered only the other one. Detailed analysis of these distributions has revealed that the ring hydrogen atoms are mainly solvated by the anions, while the methyl and butyl terminal H atoms are surrounded by like atoms. The extent of this inhomogeneity was assessed by calculating the cluster size distribution that shows that the dimers are the most abundant ones.
Cited By
This article is cited by 5 publications.
- José Enrique Vázquez-Cervantes, G. Andrés Cisneros. Development of Imidazolium-Based Parameters for AMOEBA-IL. The Journal of Physical Chemistry B 2023, 127 (24) , 5481-5493. https://doi.org/10.1021/acs.jpcb.3c00986
- Dmytro Dudariev, Volodymyr Koverga, Oleg Kalugin, François-Alexandre Miannay, Kamil Polok, Toshiyuki Takamuku, Pál Jedlovszky, Abdenacer Idrissi. Insight to the Local Structure of Mixtures of Imidazolium-Based Ionic Liquids and Molecular Solvents from Molecular Dynamics Simulations and Voronoi Analysis. The Journal of Physical Chemistry B 2023, 127 (11) , 2534-2545. https://doi.org/10.1021/acs.jpcb.2c08818
- Toshiyuki Takamuku, Atsuya Tashiro, Masahiro Kawano, Masatoshi Ando, Akira Ogawa, Koichiro Sadakane, Hiroki Iwase, Hideaki Shirota. Anion Effects on the Mixing States of 1-Methyl-3-octylimidazolium Tetrafluoroborate and Bis(trifluoromethylsulfonyl)amide with Methanol, Acetonitrile, and Dimethyl Sulfoxide on the Meso- and Microscopic Scales. The Journal of Physical Chemistry B 2021, 125 (51) , 13896-13907. https://doi.org/10.1021/acs.jpcb.1c08001
- Ekaterina A. Shelepova, Nikolai N. Medvedev. Connection between empty volume and solubility of light gases in [CnMIM][NTf2] ionic liquids. Journal of Molecular Liquids 2022, 368 , 120740. https://doi.org/10.1016/j.molliq.2022.120740
- Shiwei Zhang, Naoya Nishi, Seiji Katakura, Tetsuo Sakka. Evaluation of static differential capacitance at the [C 4 mim + ][TFSA − ]/electrode interface using molecular dynamics simulation combined with electrochemical surface plasmon resonance measurements. Physical Chemistry Chemical Physics 2021, 12 https://doi.org/10.1039/D1CP01435H