Cooperative structure of Li/Ni mixing and stacking faults for achieving high-capacity Co-free Li-rich oxides

作     者：Zhen Wu Yu-Han Zhang Hao Wang Zewen Liu Xudong Zhang Xin Dai Kunyang Zou Xiaoming Lou Xuechen Hu Lijing Ma Yan Liu Yongning Liu 

作者机构：State Key Laboratory for Mechanical Behavior of MaterialsXi’an Jiaotong UniversityXi’an 710049ShaanxiChina Qingdao Industrial Energy Storage Research InstituteQingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101ShandongChina Hefei Advanced Computing Center Operation Management Corp LtdHefei 230088AnhuiChina Center for High Performance ComputingNetwork Information CenterXi’an Jiaotong UniversityXi’an 710049ShaanxiChina Wuhan Dongfeng Motor Corporation LtdWuhan 430056HubeiChina School of Materials Science and Intelligent EngineeringNanjing UniversitySuzhou 215163JiangsuChina Key Laboratory of MEMS of the Ministry of EducationSoutheast UniversityNanjing 210096JiangsuChina International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2024年第95卷第8期

页      面：315-324,I0007页

核心收录：

学科分类：0808[工学-电气工程] 0809[工学-电子科学与技术（可授工学、理学学位）] 0817[工学-化学工程与技术] 0806[工学-冶金工程] 08[工学] 070203[理学-原子与分子物理] 0703[理学-化学] 0714[理学-统计学（可授理学、经济学学位）] 0701[理学-数学] 0702[理学-物理学] 

基　　金：financially supported by the National Natural Science Foundation of China(52202046,51602246,and 51801144) the Natural Science Foundation of Shanxi Provincial(2021JQ-034) 

主　　题：Co-free Li-rich oxides Li/Ni mixing Stacking faults Electronic structure 

摘      要：Co-free Li-rich layered oxides(LLOs)are emerging as promising cathode materials for Li-ion batteries due to their low cost and high ***,they commonly face severe structural instability and poor electrochemical activity,leading to diminished capacity and voltage ***,we introduce a Co-free LLO,Li_(1.167)Ni_(0.222)Mn_(0.611)O_(2)(Cf-L1),which features a cooperative structure of Li/Ni mixing and stacking *** structure regulates the crystal and electronic structures,resulting in a higher discharge capacity of 300.6 mA h g^(-1)and enhanced rate capability compared to the typical Co-free LLO,Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2)(Cf-Ls).Density functional theory(DFT)indicates that Li/Ni mixing in LLOs leads to increased Li-O-Li configurations and higher anionic redox activities,while stacking faults further optimize the electronic interactions of transition metal(TM)3d and non-bonding O 2p ***,stacking faults accommodate lattice strain,improving electrochemical reversibility during charge/discharge cycles,as demonstrated by the in situ XRD of Cf-L1 showing less lattice evolution than *** study offers a structured approach to developing Co-free LLOs with enhanced capacity,voltage,rate capability,and cyclability,significantly impacting the advancement of the next-generation Li-ion batteries.