Carbon dioxide in an ionic liquid: Structural and rotational dynamics
Abstract
Ionic liquids (ILs), which have widely tunable structural motifs and intermolecular interactions with solutes, have been proposed as possible carbon capture media. In order to inform the choice of an optimal ionic liquid system, it can be useful to understand the details of dynamics and interactions on fundamental time scales (femtoseconds to picoseconds) of dissolved gases, particularly carbon dioxide (CO2), within the complex solvation structures present in these uniquely organized materials. The rotational and local structural fluctuation dynamics of CO2 in the room temperature ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EmimNTf2) were investigated by using ultrafast infrared spectroscopy to interrogate the CO2 asymmetric stretch. Polarization-selective pump probe measurements yielded the orientational correlation function of the CO2 vibrational transition dipole. It was found that reorientation of the carbon dioxide occurs on 3 time scales: 0.91 ± 0.03, 8.3 ± 0.1, 54 ± 1 ps. The initial two are attributed to restricted wobbling motions originating from a gating of CO2 motions by the IL cations and anions. The final (slowest) decay corresponds to complete orientational randomization. Two-dimensional infrared vibrational echo (2D IR) spectroscopy provided information on structural rearrangements, which cause spectral diffusion, through the time dependence of the 2D line shape. Analysis of themore »
- Authors:
-
- Stanford Univ., CA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Stanford Univ., CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1468530
- Alternate Identifier(s):
- OSTI ID: 1241420
- Grant/Contract Number:
- FG03-84ER13251; FA9550-16-1-0104
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 144; Journal Issue: 10; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ionic liquids; chemical compounds and components; infrared spectroscopy; chemical elements; rotational dynamics; intermolecular forces; energy storage; covariance and correlation; molecular dynamics; stark effect
Citation Formats
Giammanco, Chiara H., Kramer, Patrick L., Yamada, Steven A., Nishida, Jun, Tamimi, Amr, and Fayer, Michael D. Carbon dioxide in an ionic liquid: Structural and rotational dynamics. United States: N. p., 2016.
Web. doi:10.1063/1.4943390.
Giammanco, Chiara H., Kramer, Patrick L., Yamada, Steven A., Nishida, Jun, Tamimi, Amr, & Fayer, Michael D. Carbon dioxide in an ionic liquid: Structural and rotational dynamics. United States. https://doi.org/10.1063/1.4943390
Giammanco, Chiara H., Kramer, Patrick L., Yamada, Steven A., Nishida, Jun, Tamimi, Amr, and Fayer, Michael D. Fri .
"Carbon dioxide in an ionic liquid: Structural and rotational dynamics". United States. https://doi.org/10.1063/1.4943390. https://www.osti.gov/servlets/purl/1468530.
@article{osti_1468530,
title = {Carbon dioxide in an ionic liquid: Structural and rotational dynamics},
author = {Giammanco, Chiara H. and Kramer, Patrick L. and Yamada, Steven A. and Nishida, Jun and Tamimi, Amr and Fayer, Michael D.},
abstractNote = {Ionic liquids (ILs), which have widely tunable structural motifs and intermolecular interactions with solutes, have been proposed as possible carbon capture media. In order to inform the choice of an optimal ionic liquid system, it can be useful to understand the details of dynamics and interactions on fundamental time scales (femtoseconds to picoseconds) of dissolved gases, particularly carbon dioxide (CO2), within the complex solvation structures present in these uniquely organized materials. The rotational and local structural fluctuation dynamics of CO2 in the room temperature ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EmimNTf2) were investigated by using ultrafast infrared spectroscopy to interrogate the CO2 asymmetric stretch. Polarization-selective pump probe measurements yielded the orientational correlation function of the CO2 vibrational transition dipole. It was found that reorientation of the carbon dioxide occurs on 3 time scales: 0.91 ± 0.03, 8.3 ± 0.1, 54 ± 1 ps. The initial two are attributed to restricted wobbling motions originating from a gating of CO2 motions by the IL cations and anions. The final (slowest) decay corresponds to complete orientational randomization. Two-dimensional infrared vibrational echo (2D IR) spectroscopy provided information on structural rearrangements, which cause spectral diffusion, through the time dependence of the 2D line shape. Analysis of the time-dependent 2D IR spectra yields the frequency-frequency correlation function (FFCF). Polarization-selective 2D IR experiments conducted on the CO2 asymmetric stretch in the parallel- and perpendicular-pumped geometries yield significantly different FFCFs due to a phenomenon known as reorientation-induced spectral diffusion (RISD), revealing strong vector interactions with the liquid structures that evolve slowly on the (independently measured) rotation time scales. To separate the RISD contribution to the FFCF from the structural spectral diffusion contribution, the previously developed first order Stark effect RISD model is reformulated to describe the second order (quadratic) Stark effect—the first order Stark effect vanishes because CO2 does not have a permanent dipole moment. Through this analysis, we characterize the structural fluctuations of CO2 in the ionic liquid solvation environment, which separate into magnitude-only and combined magnitude and directional correlations of the liquid’s time dependent electric field. This new methodology will enable highly incisive comparisons between CO2 dynamics in a variety of ionic liquid systems.},
doi = {10.1063/1.4943390},
journal = {Journal of Chemical Physics},
number = 10,
volume = 144,
place = {United States},
year = {Fri Mar 11 00:00:00 EST 2016},
month = {Fri Mar 11 00:00:00 EST 2016}
}
Web of Science
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