Highly Concentrated Asymmetric KTFSI for Aqueous Potassium Ion Batteries

Author:

Kumaresan Thileep Kumar1,Ikhe Amol Bhairuba1,Park Woon‐Bae1,Prabakar S. J. Richard1,Noh Hyeon Su1,Seo Jung Yong1,Lee Young‐Kook2,Sohn Kee‐Sun3,Kwak Joon Seop4,Pyo Myoungho4ORCID

Affiliation:

1. Department of Advanced Components and Materials Engineering Sunchon National University Chonnam 57922 Republic of Korea

2. Department of Materials Science and Engineering Yonsei University Seoul 03722 Republic of Korea

3. Faculty of Nanotechnology and Advanced Materials Engineering Sejong University Seoul 05006 Republic of Korea

4. Department of Energy Engineering Korea Institute of Energy Technology Chonnam 58330 Republic of Korea

Abstract

AbstractPotassium imide salt (KCTFSI), featuring cyano (C≡N) and trifluoromethanesulfonyl (TFSI) branches, is reported for the first time as a promising electrolyte for aqueous potassium‐ion batteries (KIBs). In contrast to the limited solubility of symmetric KTFSI (1.5m), asymmetric KCTFSI achieves a high saturation concentration of 32.2m within a “water‐in‐salt” region. Experimental and theoretical studies reveal that the remarkable enhancement of solubility is associated with the asymmetry of CTFSI anions and likely the preferential formation of contact‐ion pairs through C≡N coordination. The 32.2m KCTFSI solution not only extends the electrochemical stability window (3.80 V on Al) but also maintains a liquid state at low temperatures (−15 °C) for an extended period, in sharp contrast to the immediate solidification of potassium bis(fluorosulfonyl)imide (KFSI, 30m) and potassium trifluoromethanesulfonate (KOTF, 22m) solutions. Thanks to its wide voltage window and supercooling behavior, KCTFSI demonstrates excellent compatibility with perylene‐3,4,9,10‐tetracarboxylic diimide (PTCDI) anode and KVPO4F (or K2Fe[Fe(CN)6]·2H2O) cathode over a wide temperature range. For instance, full cells of PTCDI/KCTFSI/KVPO4F exhibit reasonable cyclability with an average discharge voltage of 1.7 V over 300 charge/discharge cycles at −15 °C. it is anticipated that this work will inspire new designs of hybrid electrolytes based on CTFSI to advance the realization of viable aqueous KIBs.

Funder

National Research Foundation of Korea

Ministry of Science and ICT, South Korea

Publisher

Wiley

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