SO2 Solvation in the 1-Ethyl-3-Methylimidazolium Thiocyanate Ionic Liquid by Incorporation into the Extended Cation–Anion Network

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• 作者：Dzmitry S. Firaha ; Mikhail Kavalchuk ; Barbara Kirchner
• 关键词：Linker effect ; Sulfur dioxide ; Ionic liquids ; Gas absorption ; Thiocyanate ; SO2 adduct ; 1 ; Ethyl ; 3 ; methylimidazolium thiocyanate
• 刊名：Journal of Solution Chemistry
• 出版年：2015
• 出版时间：April 2015
• 年：2015
• 卷：44
• 期：3-4
• 页码：838-849
• 全文大小：2,243 KB
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• 作者单位：Dzmitry S. Firaha (1)
  Mikhail Kavalchuk (1)
  Barbara Kirchner (1)
  
  1. Mulliken Center for Theoretical Chemistry, Institut für Physikalische und Theoretische Chemie, University of Bonn, Beringstra?e 4+6, Bonn, Germany
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Physical Chemistry
  Industrial Chemistry and Chemical Engineering
  Geochemistry
  Oceanography
  Inorganic Chemistry
  Condensed Matter
  
• 出版者：Springer Netherlands
• ISSN：1572-8927

文摘

We have carried out an ab initio molecular dynamics study on the sulfur dioxide (SO₂) solvation in 1-ethyl-3-methylimidazolium thiocyanate for which we have observed that both cations and anions play an essential role in the solvation of SO₂. Whereas, the anions tend to form a thiocyanate- and much less often an isothiocyanate-SO₂ adduct, the cations create a “cage-around SO₂ with those groups of atoms that donate weak interactions like the alkyl hydrogen atoms as well as the heavy atoms of the \(\pi \)-system. Despite these similarities between the solvation of SO₂ and CO₂ in ionic liquids, an essential difference was observed with respect to the acidic protons. Whereas CO₂ avoids accepting hydrogen bonds form the acidic hydrogen atoms of the cations, SO₂ can from O(SO₂)–H(cation) hydrogen bonds and thus together with the strong anion-adduct it actively integrates in the hydrogen bond network of this particular ionic liquid. The fact that SO₂ acts in this way was termed a linker effect by us, because the SO₂ can be situated between cation and anion operating as a linker between them. The particular contacts are the H(cation)\(\cdots \)O(SO₂) hydrogen bond and a S(anion)–S(SO₂) sulfur bridge. Clearly, this observation provides a possible explanation for the question of why the SO₂ solubility in these ionic liquids is so high.