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Title: Bias-Dependent Molecular-Level Structure of Electrical Double Layer in Ionic Liquid on Graphite

Abstract

Bias-dependent structure of electrochemical double layers at liquid-solid interfaces underpin a multitude of phenomena in virtually all areas of scientific enquiry ranging from energy storage and conversion systems, biology, to geophysics and geochemistry. Here we report the bias-evolution of the electric double layer structure of an ionic liquid on highly ordered pyrolytic graphite as a model system for carbon-based electrodes for electrochemical supercapacitors measured by atomic force microscopy. Matching the observed structures to molecular dynamics simulations allows us to resolve steric effects due to cation and anion layers. We observe reconfiguration under applied bias and the orientational transitions in the Stern layer. The synergy between molecular dynamics simulation and experiment provides a comprehensive picture of structural phenomena and long- and short range interactions. This insight will improve understanding of the mechanism of charge storage in electrochemical capacitors on a molecular level which can be used to enhance their electrochemical performance.

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Center for Nanophase Materials Sciences
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1110865
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nano Letters; Journal Volume: 13; Journal Issue: 12
Country of Publication:
United States
Language:
English
Subject:
atomic force microscopy; ionic liquids; electrical double layer

Citation Formats

Black, Jennifer M., Walters, Deron, Labuda, Aleksander, Feng, Guang, Hillesheim, Patrick C., Dai, Sheng, Cummings, Peter T., Kalinin, Sergei V., Proksch, Roger, and Balke, Nina. Bias-Dependent Molecular-Level Structure of Electrical Double Layer in Ionic Liquid on Graphite. United States: N. p., 2013. Web. doi:10.1021/nl4031083.
Black, Jennifer M., Walters, Deron, Labuda, Aleksander, Feng, Guang, Hillesheim, Patrick C., Dai, Sheng, Cummings, Peter T., Kalinin, Sergei V., Proksch, Roger, & Balke, Nina. Bias-Dependent Molecular-Level Structure of Electrical Double Layer in Ionic Liquid on Graphite. United States. doi:10.1021/nl4031083.
Black, Jennifer M., Walters, Deron, Labuda, Aleksander, Feng, Guang, Hillesheim, Patrick C., Dai, Sheng, Cummings, Peter T., Kalinin, Sergei V., Proksch, Roger, and Balke, Nina. Wed . "Bias-Dependent Molecular-Level Structure of Electrical Double Layer in Ionic Liquid on Graphite". United States. doi:10.1021/nl4031083.
@article{osti_1110865,
title = {Bias-Dependent Molecular-Level Structure of Electrical Double Layer in Ionic Liquid on Graphite},
author = {Black, Jennifer M. and Walters, Deron and Labuda, Aleksander and Feng, Guang and Hillesheim, Patrick C. and Dai, Sheng and Cummings, Peter T. and Kalinin, Sergei V. and Proksch, Roger and Balke, Nina},
abstractNote = {Bias-dependent structure of electrochemical double layers at liquid-solid interfaces underpin a multitude of phenomena in virtually all areas of scientific enquiry ranging from energy storage and conversion systems, biology, to geophysics and geochemistry. Here we report the bias-evolution of the electric double layer structure of an ionic liquid on highly ordered pyrolytic graphite as a model system for carbon-based electrodes for electrochemical supercapacitors measured by atomic force microscopy. Matching the observed structures to molecular dynamics simulations allows us to resolve steric effects due to cation and anion layers. We observe reconfiguration under applied bias and the orientational transitions in the Stern layer. The synergy between molecular dynamics simulation and experiment provides a comprehensive picture of structural phenomena and long- and short range interactions. This insight will improve understanding of the mechanism of charge storage in electrochemical capacitors on a molecular level which can be used to enhance their electrochemical performance.},
doi = {10.1021/nl4031083},
journal = {Nano Letters},
number = 12,
volume = 13,
place = {United States},
year = {Wed Dec 11 00:00:00 EST 2013},
month = {Wed Dec 11 00:00:00 EST 2013}
}