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Reorganizing Helmholtz Adsorption Plane Enables Sodium Layered‐Oxide Cathode beyond High Oxidation Limits

Mei‐Yan SunMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaBo LiuMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaYang XiaMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaYa‐Xuan WangMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaYin‐Qi ZhengMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaLan WangMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaLiang DengMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaLei ZhaoMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Laboratory of Space Power‐Sources Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaZhen‐Bo WangCollege of Materials Science and Engineering Shenzhen University Shenzhen Guangdong 518071 China
2024en
ABI

Аннотация

Abstract Sodium layered‐oxides (Na x TMO 2 ) sustain severe interfacial stability issues when subjected to battery applications. Particularly at high potential, the oxidation limits including transition metal dissolution and solid electrolyte interphase reformation are intertwined upon the cathode, resulting in poor cycle ability. Herein, by rearranging the complex and structure of the Helmholtz absorption plane adjacent to Na x TMO 2 cathodes, the mechanism of constructing stable cathode/electrolyte interphase (CEI) to push up oxidation limits is clarified. The strong absorbent fluorinated anions replace the solvents into the inner Helmholtz plane, thereby reorganizing the Helmholtz absorption structure and spontaneously inducing anion‐dominated interphase to envelop more active sites for layered oxides. More importantly, such multi‐component CEI proves effective for the long‐term durability of a series of manganese‐based oxide cathodes, which achieves a 1500‐cycles lifetime against high oxidation voltage limit beyond 4.3 V. This work unravels the key role of breaking high‐oxidation limits in attaining higher energy density of layered‐oxide systems.

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