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Comparative Internal Pressure Evolution at Interfaces of Activated Carbon for Supercapacitors Containing Electrolytes Based on Linear and Cyclic Ammonium Tetrafluoroborate Salts in Acetonitrile

Nikiforidis, Georgios; Phadke, Satyajit; Anouti, Meriem; (2022) Comparative Internal Pressure Evolution at Interfaces of Activated Carbon for Supercapacitors Containing Electrolytes Based on Linear and Cyclic Ammonium Tetrafluoroborate Salts in Acetonitrile. Advanced Materials Interfaces 10.1002/admi.202202046. (In press). Green open access

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Abstract

In this study, the real-time increase in pressure of the accumulated gases at the electrode/electrolyte interface serves as a safety criterion for four conductive electrolytes comprising acetonitrile (ACN) and organic salts. They include tetrafluoroborate as an anion and cyclic 1,1-dimethylpyrrolidinium (Pyr11+), spiro-(1,1′)-bipyrrolidinium (SBP+), acyclic methyl triethyl ammonium (Et3MeN+) or standard tetraethylammonium (Et4N+) as cations. The main focus lies on the SPBF4/ACN system. While the concentrated Pyr11BF4/ACN exhibits a minimal pressure evolution (≈25 Pa) under ambient conditions at 3.0 V, its electrochemical stability is inferior to SPBF4 at high operating voltage. The electrolytes with acyclic tetrafluoroborate salts (1.0 mol L−1) reveal a 20-fold increase in pressure due to the weak salt-ACN interactions and the subsequent high solvent evaporation. The pressure evolution at the interface of activated carbon/electrolyte in electrochemical double layer capacitor (EDLCs) is merely related to the operating voltage and cation nature, viz. Pyr11+ < SBP+ < Et4N+ < Et3MeN+. The fixed specific capacity of 109 F g−1, volumetric capacity of 76 F cm−3, and moderate gas generation (≈190 Pa at 3.0 V, that shifts to ≈400 Pa at 3.4 V) confirm the safe character of the SPBF4/ACN electrolyte for such energy storage devices.

Type: Article
Title: Comparative Internal Pressure Evolution at Interfaces of Activated Carbon for Supercapacitors Containing Electrolytes Based on Linear and Cyclic Ammonium Tetrafluoroborate Salts in Acetonitrile
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/admi.202202046
Publisher version: https://doi.org/10.1002/admi.202202046
Language: English
Additional information: © 2022 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/).
Keywords: acetonitrile, activated carbon, EDLC, gas formation, ionicity, spiro
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > MAPS Faculty Office > Institute for Materials Discovery
URI: https://discovery.ucl.ac.uk/id/eprint/10162192
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