Functionalization of Electrodes with Tunable [EMIM]x[Cl]x+1– Ionic Liquid Clusters for Electrochemical Separations
Abstract
Functionalization of electrodes with clusters of hydrophobic molecules may improve the energy efficiency and selectivity of electrochemical separations by modulating the desolvation process occurring at the interface. Ionic liquids (IL), which have a broad range of compositions and properties, are potential candidates for controlling the transport, desolvation, and adsorption of target ions at electrochemical interfaces. We report a joint experimental and theoretical investigation of the structure, stability, and selective adsorption properties of the IL clusters 1-ethyl-3-methylimidazolium chloride [EMIM]x[Cl]x+1- (x = 1 – 10) and demonstrate their ability to adsorb and separate ions from solution. The structure and stability of the IL clusters are determined experimentally using high-mass-resolution electrospray ionization mass spectrometry, collision-induced dissociation, and negative ion photoelectron spectroscopy. Global optimization theory and ab initio molecular dynamics simulations provide molecular-level insight into the bonding and structural fluxionality of these species. Ion soft landing is used to selectively functionalize the surface of highly oriented pyrolytic graphite (HOPG) working electrodes with [EMIM]1[Cl]2-, [EMIM]3[Cl]4-, and [EMIM]5[Cl]6- clusters. Kelvin probe microscopy provides insight into the relative stability of the clusters on HOPG and their effect on the work function of IL-functionalized electrodes. Cyclic voltammetry measurements reveal irreversible adsorption of Fe(CN)64-/3- anions during redox cycling, whilemore »
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1970130
- Report Number(s):
- PNNL-SA-168307
Journal ID: ISSN 0897-4756
- Grant/Contract Number:
- AC05-76RL01830; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 6; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; anions; cluster chemistry; cluster ions; electrodes; ions
Citation Formats
Baxter, Eric T., Zhang, Jun, Tan, Shuai, Nguyen, Manh-Thuong, Zhang, Difan, Yuan, Qinqin, Cao, Wenjin, Wang, Xue-Bin, Prabhakaran, Venkateshkumar, Glezakou, Vassiliki-Alexandra, and Johnson, Grant E. Functionalization of Electrodes with Tunable [EMIM]x[Cl]x+1– Ionic Liquid Clusters for Electrochemical Separations. United States: N. p., 2022.
Web. doi:10.1021/acs.chemmater.1c03836.
Baxter, Eric T., Zhang, Jun, Tan, Shuai, Nguyen, Manh-Thuong, Zhang, Difan, Yuan, Qinqin, Cao, Wenjin, Wang, Xue-Bin, Prabhakaran, Venkateshkumar, Glezakou, Vassiliki-Alexandra, & Johnson, Grant E. Functionalization of Electrodes with Tunable [EMIM]x[Cl]x+1– Ionic Liquid Clusters for Electrochemical Separations. United States. https://doi.org/10.1021/acs.chemmater.1c03836
Baxter, Eric T., Zhang, Jun, Tan, Shuai, Nguyen, Manh-Thuong, Zhang, Difan, Yuan, Qinqin, Cao, Wenjin, Wang, Xue-Bin, Prabhakaran, Venkateshkumar, Glezakou, Vassiliki-Alexandra, and Johnson, Grant E. Mon .
"Functionalization of Electrodes with Tunable [EMIM]x[Cl]x+1– Ionic Liquid Clusters for Electrochemical Separations". United States. https://doi.org/10.1021/acs.chemmater.1c03836. https://www.osti.gov/servlets/purl/1970130.
@article{osti_1970130,
title = {Functionalization of Electrodes with Tunable [EMIM]x[Cl]x+1– Ionic Liquid Clusters for Electrochemical Separations},
author = {Baxter, Eric T. and Zhang, Jun and Tan, Shuai and Nguyen, Manh-Thuong and Zhang, Difan and Yuan, Qinqin and Cao, Wenjin and Wang, Xue-Bin and Prabhakaran, Venkateshkumar and Glezakou, Vassiliki-Alexandra and Johnson, Grant E.},
abstractNote = {Functionalization of electrodes with clusters of hydrophobic molecules may improve the energy efficiency and selectivity of electrochemical separations by modulating the desolvation process occurring at the interface. Ionic liquids (IL), which have a broad range of compositions and properties, are potential candidates for controlling the transport, desolvation, and adsorption of target ions at electrochemical interfaces. We report a joint experimental and theoretical investigation of the structure, stability, and selective adsorption properties of the IL clusters 1-ethyl-3-methylimidazolium chloride [EMIM]x[Cl]x+1- (x = 1 – 10) and demonstrate their ability to adsorb and separate ions from solution. The structure and stability of the IL clusters are determined experimentally using high-mass-resolution electrospray ionization mass spectrometry, collision-induced dissociation, and negative ion photoelectron spectroscopy. Global optimization theory and ab initio molecular dynamics simulations provide molecular-level insight into the bonding and structural fluxionality of these species. Ion soft landing is used to selectively functionalize the surface of highly oriented pyrolytic graphite (HOPG) working electrodes with [EMIM]1[Cl]2-, [EMIM]3[Cl]4-, and [EMIM]5[Cl]6- clusters. Kelvin probe microscopy provides insight into the relative stability of the clusters on HOPG and their effect on the work function of IL-functionalized electrodes. Cyclic voltammetry measurements reveal irreversible adsorption of Fe(CN)64-/3- anions during redox cycling, while electrochemical impedance spectroscopy indicates a substantial decrease in the electron transfer resistance of the IL-functionalized electrodes due to adsorption of Fe(CN)64-/3-. Overall, our findings demonstrate that IL clusters with different size and stoichiometry may be used to increase the efficiency of electrochemical separations, opening new horizons in selective electrode functionalization.},
doi = {10.1021/acs.chemmater.1c03836},
journal = {Chemistry of Materials},
number = 6,
volume = 34,
place = {United States},
year = {Mon Feb 28 00:00:00 EST 2022},
month = {Mon Feb 28 00:00:00 EST 2022}
}
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