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reversible cationic-anionic redox in disordered rocksalt cathodes enabled by fluorination-induced integrated structure design

引用

Journal of Energy Chemistry 2023年第7期82卷 158-169,I0004页

作者： Feng Wu Jinyang Dong Jiayu Zhao Qi Shi Yun Lu Ning Li Duanyun Cao Wenbo Li Jianan Hao Yu Zheng Lai Chen Yuefeng Su School of Materials Science and Engineering Beijing Key Laboratory of Environmental Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Institute of Technology Chongqing Innovation Center Chongqing 401120China BTR New Material Group Co. LtdShenzhen 518000GuangdongChina

Cation-disordered rocksalt oxides(DRX)have been identified as promising cathode materials for high energy density applications owing to their variable elemental composition and cationic-anionic redox activity.However,their practical implementation has been impeded by unwanted phenomena such as irrepressible transition metal migration/dissolution and O_(2)/CO_(2)evolution,which arise due to parasitic reactions and densification-degradation mechanisms during extended cycling.To address these issues,a micron-sized DRX cathode Li_(1.2)Ni_(1/3)Ti_(1/3)W_(2/15)O_(1.85)F_(0.15)(SLNTWOF)with F substitution and ultrathin LiF coating layer is developed by alcohols assisted sol-gel method.Within this fluorination-induced integrated structure design(FISD)strategy,in-situ F substitution modifies the activity/reversibility of the cationic-anionic redox reaction,while the ultrathin LiF coating and single-crystal structure synergistically mitigate the cathode/electrolyte parasitic reaction and densification-degradation mechanism.Attributed to the multiple modifications and size effect in the FISD strategy,the SLNTWOF sample exhibits reversible cationic-anionic redox chemistry with a meliorated reversible capacity of 290.3 mA h g^(-1)at 0.05C(1C=200 mA g^(-1)),improved cycling stability of 78.5%capacity retention after 50 cycles at 0.5 C,and modified rate capability of 102.8 mA h g^(-1)at 2 C.This work reveals that the synergistic effects between bulk structure modification,surface regulation,and engineering particle size can effectively modulate the distribution and evolution of cationic-anionic redox activities in DRX cathodes.

关键词： Cation-disordered rocksalt oxides Fluorine substitution Ultrathin LiF coating Micron-sized single-crystal reversible cationic-anionic redox

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