Affiliation:
1. Sauvage Laboratory for Smart Materials Shenzhen Key Laboratory of Flexible Printed Electronics Technology School of Materials Science and Engineering State Key Laboratory of Advanced Welding and Joining Harbin Institute of Technology (Shenzhen) 518055 Shenzhen China
2. School of Chemical Engineering The University of Adelaide 5005 Adelaide Australia
3. Key Laboratory of Radiation Physics and Technology of Ministry of Education Institute of Nuclear Science and Technology Sichuan University 610064 Chengdu China
4. Department of Materials Science and Engineering City University of Hong Kong 999077 Hong Kong China
Abstract
AbstractThe extensively studied Prussian blue analogs (PBAs) in various batteries are limited by their low discharge capacity, or subpar rate etc., which are solely reliant on the cation (de)intercalation mechanism. In contrast to the currently predominant focus on cations, we report the overlooked anion‐cation competition chemistry (Cl−, K+, Zn2+) stimulated by high‐voltage scanning. With our designed anion‐cation combinations, the KFeMnHCF cathode battery delivers comprehensively superior discharge performance, including voltage plateau >2.0 V (vs. Zn/Zn2+), capacity >150 mAh g−1, rate capability with capacity maintenance above 96 % from 0.6 to 5 A g−1, and cyclic stability exceeding 3000 cycles. We further verify that such comprehensive improvement of electrochemical performance utilizing anion‐cation competition chemistry is universal for different types of PBAs. Our work would pave a new and efficient road towards the next‐generation high‐performance PBAs cathode batteries.