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Title: Time-dependent density functional theory for the charging kinetics of electric double layer containing room-temperature ionic liquids

Abstract

Understanding the charging kinetics of electric double layers is of fundamental importance for the design and development of novel electrochemical devices such as supercapacitors and field-effect transistors. In this paper, we study the dynamic behavior of room-temperature ionic liquids using a classical time-dependent density functional theory that accounts for the molecular excluded volume effects, the electrostatic correlations, and the dispersion forces. While the conventional models predict a monotonic increase of the surface charge with time upon application of an electrode voltage, our results show that dispersion between ions results in a non-monotonic increase of the surface charge with the duration of charging. Finally and furthermore, we investigate the effects of van der Waals attraction between electrode/ionic-liquid interactions on the charging processes.

Authors:
 [1];  [2];  [1];  [1];  [3]
+ Show Author Affiliations
  1. East China Univ. of Science and Technology, Shanghai (China). School of Chemistry and Molecular Engineering. State Key Lab. of Chemical Engineering
  2. (United States). Dept. of Chemical and Environmental Engineering
  3. Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering
Publication Date:
Research Org.:
Univ. of California, Riverside, CA (United States); East China Univ. of Science and Technology, Shanghai (China); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); 111 Project of China; Chinese Scholarship Council
OSTI Identifier:
1340469
Alternate Identifier(s):
OSTI ID: 1333764
Grant/Contract Number:  
AC05-00OR22725; 91334203; B08021; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 20; 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; double layers; surface charge; electrodes; electrostatics; ionic liquids

Citation Formats

Lian, Cheng, Univ. of California, Riverside, CA, Zhao, Shuangliang, Liu, Honglai, and Wu, Jianzhong. Time-dependent density functional theory for the charging kinetics of electric double layer containing room-temperature ionic liquids. United States: N. p., 2016. Web. doi:10.1063/1.4968037.
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Lian, Cheng, Univ. of California, Riverside, CA, Zhao, Shuangliang, Liu, Honglai, & Wu, Jianzhong. Time-dependent density functional theory for the charging kinetics of electric double layer containing room-temperature ionic liquids. United States. https://doi.org/10.1063/1.4968037
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Lian, Cheng, Univ. of California, Riverside, CA, Zhao, Shuangliang, Liu, Honglai, and Wu, Jianzhong. Tue . "Time-dependent density functional theory for the charging kinetics of electric double layer containing room-temperature ionic liquids". United States. https://doi.org/10.1063/1.4968037. https://www.osti.gov/servlets/purl/1340469.
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@article{osti_1340469,
title = {Time-dependent density functional theory for the charging kinetics of electric double layer containing room-temperature ionic liquids},
author = {Lian, Cheng and Univ. of California, Riverside, CA and Zhao, Shuangliang and Liu, Honglai and Wu, Jianzhong},
abstractNote = {Understanding the charging kinetics of electric double layers is of fundamental importance for the design and development of novel electrochemical devices such as supercapacitors and field-effect transistors. In this paper, we study the dynamic behavior of room-temperature ionic liquids using a classical time-dependent density functional theory that accounts for the molecular excluded volume effects, the electrostatic correlations, and the dispersion forces. While the conventional models predict a monotonic increase of the surface charge with time upon application of an electrode voltage, our results show that dispersion between ions results in a non-monotonic increase of the surface charge with the duration of charging. Finally and furthermore, we investigate the effects of van der Waals attraction between electrode/ionic-liquid interactions on the charging processes.},
doi = {10.1063/1.4968037},
journal = {Journal of Chemical Physics},
number = 20,
volume = 145,
place = {United States},
year = {Tue Nov 29 00:00:00 EST 2016},
month = {Tue Nov 29 00:00:00 EST 2016}
}
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https://doi.org/10.1063/1.4968037
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