Journal
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
Volume 819, Issue -, Pages 347-358Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.jelechem.2017.11.005
Keywords
Room temperature ionic liquids; Mean-field; Temperature; Differential capacitance
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Funding
- National Natural Science Foundation of China [51406060]
- Shenzhen Basic Research Project [JCYJ20170307171511292]
- Centre for Doctoral Training on Theory and Simulation of Materials at Imperial College London - EPSRC [EP/L015579/1]
- Thomas Young Centre [TYC-101]
- EPSRC [EP/H004319/1] Funding Source: UKRI
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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.
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