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Title: Understanding the Mechanism of CO 2 Capture by 1,3 Di-substituted Imidazolium Acetate Based Ionic Liquids

Abstract

Efficient CO 2 capture by ionic liquids needs a thorough understanding of underlying mechanisms of the CO 2 interaction with ionic liquids, especially when it involves chemisorption. In this work we have systematically investigated the mechanism of CO 2 capture by 1,3 di-substituted imidazolium acetate ionic liquids using density functional theory. Solvent effects are analyzed using QM/MM and QM/QM approaches with the help of molecular dynamics simulations and ONIOM methods. The investigation of different stepwise mechanisms shows that CO 2 could be involved in the first step of the reaction mechanism, also a new two-step mechanism is proposed. Furthermore, the final stabilization step is analyzed and pointed out to be responsible for important experimentally-observed features of the reaction.

Authors:
 [1];  [2];  [3];  [3];  [3];  [1]
  1. Univ. of Pittsburgh, Pittsburgh, PA (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States)
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1483263
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 18; Journal Issue: 3; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mao, James X., Steckel, Janice A., Yan, Fangyong, Dhumal, Nilesh, Kim, Hyung, and Damodaran, Krishnan. Understanding the Mechanism of CO2 Capture by 1,3 Di-substituted Imidazolium Acetate Based Ionic Liquids. United States: N. p., 2015. Web. doi:10.1039/c5cp05713b.
Mao, James X., Steckel, Janice A., Yan, Fangyong, Dhumal, Nilesh, Kim, Hyung, & Damodaran, Krishnan. Understanding the Mechanism of CO2 Capture by 1,3 Di-substituted Imidazolium Acetate Based Ionic Liquids. United States. doi:10.1039/c5cp05713b.
Mao, James X., Steckel, Janice A., Yan, Fangyong, Dhumal, Nilesh, Kim, Hyung, and Damodaran, Krishnan. Wed . "Understanding the Mechanism of CO2 Capture by 1,3 Di-substituted Imidazolium Acetate Based Ionic Liquids". United States. doi:10.1039/c5cp05713b. https://www.osti.gov/servlets/purl/1483263.
@article{osti_1483263,
title = {Understanding the Mechanism of CO2 Capture by 1,3 Di-substituted Imidazolium Acetate Based Ionic Liquids},
author = {Mao, James X. and Steckel, Janice A. and Yan, Fangyong and Dhumal, Nilesh and Kim, Hyung and Damodaran, Krishnan},
abstractNote = {Efficient CO2 capture by ionic liquids needs a thorough understanding of underlying mechanisms of the CO2 interaction with ionic liquids, especially when it involves chemisorption. In this work we have systematically investigated the mechanism of CO2 capture by 1,3 di-substituted imidazolium acetate ionic liquids using density functional theory. Solvent effects are analyzed using QM/MM and QM/QM approaches with the help of molecular dynamics simulations and ONIOM methods. The investigation of different stepwise mechanisms shows that CO2 could be involved in the first step of the reaction mechanism, also a new two-step mechanism is proposed. Furthermore, the final stabilization step is analyzed and pointed out to be responsible for important experimentally-observed features of the reaction.},
doi = {10.1039/c5cp05713b},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 3,
volume = 18,
place = {United States},
year = {2015},
month = {12}
}

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Cited by: 15 works
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Works referenced in this record:

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