Achievable dual-strategy to stabilize Li-rich layered oxide interface by a one-step wet chemical reaction towards long oxygen redox reversibility  

作　　者：Bin He Yujie Dai Shuai Jiang Dawei Chen Xilong Wang Jie Song Dan Xiao Qian Zhao Yan Meng Wei Feng 

机构地区：[1]School of Mechanical Engineering,Chengdu University,Chengdu 610106,Sichuan,China [2]Institute of New Energy and Low-Carbon Technology,Sichuan University,Chengdu 610065,Sichuan,China [3]Chongqing Institute of Metrology and Quality Inspection,Chongqing 401121,China

出　　处：《Journal of Energy Chemistry》2025年第2期120-131,I0004,共13页能源化学(英文版)

基　　金：financially supported by the National Natural Science Foundation of China(No.12304077);the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224);Sichuan Science and Technology Program(No.2024NSFSC0989);the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03);the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01);the National Innovation Practice Project(No.202411079005S).

摘　　要：Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.

关 键 词：Lithium-rich layered oxide cathode One-step wet chemical reaction Surface coating Local gradient doping Interfacial oxygen 

分 类 号：TG1[金属学及工艺—金属学]