Anion-Cation Competition Chemistry for Comprehensive High-Performance Prussian Blue Analogs Cathodes

Mangwei Cui; Yilong Zhu; Hao Lei; Ao Liu; Funian Mo; Kefeng Ouyang; Sheng Chen; Xi Lin; Zuhuang Chen; Kaikai Li; Yan Jiao; Chunyi Zhi; Yan Huang

doi:10.1002/anie.202405428

Anion-Cation Competition Chemistry for Comprehensive High-Performance Prussian Blue Analogs Cathodes

Angew Chem Int Ed Engl. 2024 Jun 3;63(23):e202405428. doi: 10.1002/anie.202405428. Epub 2024 Apr 19.

Authors

Mangwei Cui¹, Yilong Zhu², Hao Lei¹, Ao Liu¹, Funian Mo¹, Kefeng Ouyang¹, Sheng Chen³, Xi Lin¹, Zuhuang Chen¹, Kaikai Li¹, Yan Jiao², Chunyi Zhi⁴, Yan Huang¹

Affiliations

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.

PMID: 38563631
DOI: 10.1002/anie.202405428

Abstract

The 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.

Keywords: PBAs cathode batteries; anion-cation competition chemistry; electrochemical performance.

Abstract

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