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Title: Two coexisting liquid phases in switchable ionic liquids

Abstract

Switchable ionic liquids (SWILs) derived from organic bases and alcohols are attractive due to their applications in gas capture, separations, and nanomaterial synthesis. However, their exact solvent structure still remains a mystery. Here, we present the first chemical mapping of a SWIL solvent structure using in situ time-of-flight secondary ion mass spectrometry. In situ chemical mapping discovers two coexisting liquid phases and molecular structures vastly different from conventional ionic liquids. SWIL chemical speciation is found to be more complex than the known stoichiometry. Dimers and ionic clusters have been identified in SIMS spectra; and confirmed to be the chemical species differentiating from non-ionic liquids via spectral principal component analysis. Our unique in situ molecular imaging has advanced the understanding of SWIL chemistry and how this “heterogeneous” liquid structure may impact SWILs’ physical and thermodynamic properties and associated applications.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Earth and Biological Sciences Directorate
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). W. R. Wiley Environmental Molecular Science Lab.
  4. Idaho State Univ., Pocatello, ID (United States). Dept. Chemistry
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1464143
Report Number(s):
PNNL-SA-122167
Journal ID: ISSN 1463-9076; PPCPFQ; ark:/13030/qt1fd6j94m
Grant/Contract Number:  
AC02-05CH11231; AC05-76RL01830
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: 19; Journal Issue: 34; Related Information: © 2017 the Owner Societies.; 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

Yao, Juan, Lao, David B., Sui, Xiao, Zhou, Yufan, Nune, Satish K., Ma, Xiang, Troy, Tyler P., Ahmed, Musa, Zhu, Zihua, Heldebrant, David J., and Yu, Xiao-Ying. Two coexisting liquid phases in switchable ionic liquids. United States: N. p., 2017. Web. doi:10.1039/c7cp03754f.
Yao, Juan, Lao, David B., Sui, Xiao, Zhou, Yufan, Nune, Satish K., Ma, Xiang, Troy, Tyler P., Ahmed, Musa, Zhu, Zihua, Heldebrant, David J., & Yu, Xiao-Ying. Two coexisting liquid phases in switchable ionic liquids. United States. doi:10.1039/c7cp03754f.
Yao, Juan, Lao, David B., Sui, Xiao, Zhou, Yufan, Nune, Satish K., Ma, Xiang, Troy, Tyler P., Ahmed, Musa, Zhu, Zihua, Heldebrant, David J., and Yu, Xiao-Ying. Fri . "Two coexisting liquid phases in switchable ionic liquids". United States. doi:10.1039/c7cp03754f. https://www.osti.gov/servlets/purl/1464143.
@article{osti_1464143,
title = {Two coexisting liquid phases in switchable ionic liquids},
author = {Yao, Juan and Lao, David B. and Sui, Xiao and Zhou, Yufan and Nune, Satish K. and Ma, Xiang and Troy, Tyler P. and Ahmed, Musa and Zhu, Zihua and Heldebrant, David J. and Yu, Xiao-Ying},
abstractNote = {Switchable ionic liquids (SWILs) derived from organic bases and alcohols are attractive due to their applications in gas capture, separations, and nanomaterial synthesis. However, their exact solvent structure still remains a mystery. Here, we present the first chemical mapping of a SWIL solvent structure using in situ time-of-flight secondary ion mass spectrometry. In situ chemical mapping discovers two coexisting liquid phases and molecular structures vastly different from conventional ionic liquids. SWIL chemical speciation is found to be more complex than the known stoichiometry. Dimers and ionic clusters have been identified in SIMS spectra; and confirmed to be the chemical species differentiating from non-ionic liquids via spectral principal component analysis. Our unique in situ molecular imaging has advanced the understanding of SWIL chemistry and how this “heterogeneous” liquid structure may impact SWILs’ physical and thermodynamic properties and associated applications.},
doi = {10.1039/c7cp03754f},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 34,
volume = 19,
place = {United States},
year = {2017},
month = {6}
}

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Works referenced in this record:

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