Enhancing the Capacitive Performance of Electric Double-Layer Capacitors with Ionic Liquid Mixtures

Lian, C.; Liu, K.; Van Aken, Katherine L.; Gogotsi, Yury G.; Wesolowski, David J.; Liu, Honglai; Jiang, D. E.; Wu, Jianzhong

doi:10.1021/acsenergylett.6b00010

Title: Enhancing the Capacitive Performance of Electric Double-Layer Capacitors with Ionic Liquid Mixtures

Journal Article · Mon Apr 18 00:00:00 EDT 2016 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.6b00010· OSTI ID:1346631

Lian, C. ^[1]; Liu, K. ^[2]; Van Aken, Katherine L. ^[3]; Gogotsi, Yury G. ^[3]; Wesolowski, David J. ^[4]; Liu, Honglai ^[5]; Jiang, D. E. ^[6]; Wu, Jianzhong ^[2]

Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering; East China Univ. of Science and Technology, Shanghai (China). State Key Lab. of Chemical Engineering
Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering
Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineering. A.J. Drexel Nanomaterials Inst.
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
East China Univ. of Science and Technology, Shanghai (China). State Key Lab. of Chemical Engineering
Univ. of California, Riverside, CA (United States). Dept. of Chemistry

Formulating room-temperature ionic liquid (RTIL) mixed electrolytes was recently proposed as an effective and convenient strategy to increase the capacitive performance of electrochemical capacitors. In this paper, we investigate the electrical double-layer (EDL) structure and the capacitance of two RTILs, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMI-TFSI) and 1-ethyl-3-methylimidazolium tetrafluoroborate (EMI-BF₄), and their mixtures with onion-like carbon electrodes using experiment and classical density functional theory. The principal difference between these ionic liquids is the smaller diameter of the BF₄^– anion relative to the TFSI^– anion and the EMI⁺ cation. A volcano-shaped trend is identified for the capacitance versus the composition of the RTIL mixture. The mixture effect, which makes more counterions pack on and more co-ions leave from the electrode surface, leads to an increase of the counterion density within the EDL and thus a larger capacitance. Finally, these theoretical predictions are in good agreement with our experimental observations and offer guidance for designing RTIL mixtures for EDL supercapacitors.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, Riverside, CA (United States); East China Univ. of Science and Technology, Shanghai (China); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Chinese Scholarship Council

Contributing Organization:: Drexel Univ., Philadelphia, PA (United States)

Grant/Contract Number:: AC05-00OR22725; 91334203; 21376074; B08021

OSTI ID:: 1346631

Journal Information:: ACS Energy Letters, Vol. 1, Issue 1; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 117 works

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