On the temperature dependence of the double layer capacitance of ionic liquids.
File(s)TDP_AC_4.pdf (1.02 MB)
Accepted version
Author(s)
Chen, Ming
Goodwin, Zachary AH
Feng, Guang
Kornyshev, Alexei A
Type
Journal Article
Abstract
The temperature dependence of room temperature ionic liquids differential capacitance is studied here with both theoretical and computational methods. On the theory front, the lattice-gas mean-field theory of ionic liquids is further generalised to account for ‘ion pairing’ and ‘neutral aggregate’ formation. An anomalous temperature dependence of linear response capacitance was found, similar to that reported in earlier work. The theory also predicted that differential capacitance curves transform from a camel to bell shape with increasing temperature. Molecular dynamics simulations verified the expected transition in shape of differential capacitance curves with temperature and the dependence of linear response capacitance on temperature. Further investigation into charge density distributions revealed an ordered structure, reminiscent of oriented ion pairs and neutral aggregates, extending far enough from the electrode to control the capacitance-voltage response. It was found that these structures were dismantled with increasing temperature, as predicted by the mean-field theory.
Date Issued
2017-11-08
Date Acceptance
2017-11-02
Citation
Journal of Electroanalytical Chemistry, 2017, 819, pp.347-358
ISSN
1572-6657
Publisher
Elsevier
Start Page
347
End Page
358
Journal / Book Title
Journal of Electroanalytical Chemistry
Volume
819
Copyright Statement
© 2017 Elsevier Ltd. All rights reserved. This manuscript is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International Licence http://creativecommons.org/licenses/by-nc-nd/4.0/
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000435619700046&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Chemistry, Analytical
Electrochemistry
Chemistry
Room temperature ionic liquids
Mean-field
Temperature
Differential capacitance
ELECTRICAL DOUBLE-LAYER
MOLECULAR-DYNAMICS SIMULATION
RESTRICTED PRIMITIVE MODEL
FIELD-THEORETICAL APPROACH
MONTE-CARLO-SIMULATION
DIFFERENTIAL CAPACITANCE
ELECTROLYTE-SOLUTIONS
HOLE THEORY
INTERFACIAL STRUCTURE
TRANSPORT-PROPERTIES
Publication Status
Published