Reaction Ensemble Monte Carlo Simulations of CO2 Absorption in the Reactive Ionic Liquid Triethyl(octyl)phosphonium 2-Cyanopyrrolide
Abstract
The absorption of CO2 into an aprotic heterocyclic anion ionic liquid (IL) is modeled here using reaction ensemble Monte Carlo (RxMC) with the semigrand reaction move. RxMC has previously been unable to sample chemical equilibrium involving molecular ions in nanostructured liquids due to the high free-energy requirements to open and close cavities and restructure the surrounding environment. Our results are validated by experiments in the modeled IL, triethyl(octyl)phosphonium 2-cyanopyrrolide ([P2228][cnp]), and in a close analog with longer alkyl chains on the cation. Heats of absorption and reaction from both experiment and simulation are exothermic and of comparable magnitude. Replacing experimental Henry’s constants with their simulated counterparts improves the accuracy of a Langmuir-type model at moderate pressures. Nonidealities that affect chemical equilibrium are identified and calculated with high precision.
- Authors:
-
[1];
[2];
[3]
- Univ. of Notre Dame, IN (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
- Univ. of Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry
- Univ. of Notre Dame, IN (United States). Dept. of Chemical and Biomolecular Engineering
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of Notre Dame, IN (United States)
- Sponsoring Org.:
- USDOE; US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
- OSTI Identifier:
- 1512630
- Report Number(s):
- LLNL-JRNL-754884
Journal ID: ISSN 1948-7185; 939774
- Grant/Contract Number:
- AC52-07NA27344; FA9550-18-1-0321; CHE-1565471
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 18; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Mullen, Ryan Gotchy, Corcelli, Steven A., and Maginn, Edward J. Reaction Ensemble Monte Carlo Simulations of CO2 Absorption in the Reactive Ionic Liquid Triethyl(octyl)phosphonium 2-Cyanopyrrolide. United States: N. p., 2018.
Web. doi:10.1021/acs.jpclett.8b02304.
Mullen, Ryan Gotchy, Corcelli, Steven A., & Maginn, Edward J. Reaction Ensemble Monte Carlo Simulations of CO2 Absorption in the Reactive Ionic Liquid Triethyl(octyl)phosphonium 2-Cyanopyrrolide. United States. https://doi.org/10.1021/acs.jpclett.8b02304
Mullen, Ryan Gotchy, Corcelli, Steven A., and Maginn, Edward J. Thu .
"Reaction Ensemble Monte Carlo Simulations of CO2 Absorption in the Reactive Ionic Liquid Triethyl(octyl)phosphonium 2-Cyanopyrrolide". United States. https://doi.org/10.1021/acs.jpclett.8b02304. https://www.osti.gov/servlets/purl/1512630.
@article{osti_1512630,
title = {Reaction Ensemble Monte Carlo Simulations of CO2 Absorption in the Reactive Ionic Liquid Triethyl(octyl)phosphonium 2-Cyanopyrrolide},
author = {Mullen, Ryan Gotchy and Corcelli, Steven A. and Maginn, Edward J.},
abstractNote = {The absorption of CO2 into an aprotic heterocyclic anion ionic liquid (IL) is modeled here using reaction ensemble Monte Carlo (RxMC) with the semigrand reaction move. RxMC has previously been unable to sample chemical equilibrium involving molecular ions in nanostructured liquids due to the high free-energy requirements to open and close cavities and restructure the surrounding environment. Our results are validated by experiments in the modeled IL, triethyl(octyl)phosphonium 2-cyanopyrrolide ([P2228][cnp]), and in a close analog with longer alkyl chains on the cation. Heats of absorption and reaction from both experiment and simulation are exothermic and of comparable magnitude. Replacing experimental Henry’s constants with their simulated counterparts improves the accuracy of a Langmuir-type model at moderate pressures. Nonidealities that affect chemical equilibrium are identified and calculated with high precision.},
doi = {10.1021/acs.jpclett.8b02304},
journal = {Journal of Physical Chemistry Letters},
number = 18,
volume = 9,
place = {United States},
year = {Thu Aug 23 00:00:00 EDT 2018},
month = {Thu Aug 23 00:00:00 EDT 2018}
}
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