Enhancing thermodynamic stability of single-crystal Ni-rich cathode material via a synergistic dual-substitution strategy  

作　　者：Jixue Shen Hui Li Haoyu Qi Zhan Lin Zeheng Li Chuanbo Zheng Weitong Du Hao Chen Shanqing Zhang 

机构地区：[1]School of Metallurgy Engineering,Jiangsu University of Science and Technology,Zhangjiagang 215600,Jiangsu,China [2]School of Metallurgy and Environment,Central South University,Changsha 410083,Hunan,China [3]Guangdong Laboratory of Chemistry and Fine Chemical Industry Jieyang Center,Jieyang 515200,Guangdong,China [4]Institute of Sustainable Transformation,School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou 510006,Guangdong,China [5]Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,Zhejiang,China [6]Centre for Catalysis and Clean Energy,School of Environment and Science,Gold Coast Campus,Griffith University,Gold Coast 4222,Queensland,Australia

出　　处：《Journal of Energy Chemistry》2024年第1期428-436,I0010,共10页能源化学（英文版）

基　　金：financially supported by the Natural Science Foundation of Jiangsu Province,China (BK20210887);the Jiangsu Provincial Double Innovation Program,China (JSSCB20210984);the Natural Science Fund for Colleges and Universities of Jiangsu Province,China (21KJB450003);the Jiangsu University of Science and Technology Doctoral Research Start-up Fund,China (120200012)。

摘　　要：Nickel(Ni)-rich cathode materials have become promising candidates for the next-generation electrical vehicles due to their high specific capacity.However,the poor thermodynamic stability(including cyclic performance and safety performance or thermal stability)will restrain their wide commercial application.Herein,a single-crystal Ni-rich Li Ni_(0.83)Co_(0.12)Mn_(0.05)O_(2) cathode material is synthesized and modified by a dual-substitution strategy in which the high-valence doping element improves the structural stability by forming strong metal–oxygen binding forces,while the low-valence doping element eliminates high Li^(+)/Ni^(2+)mixing.As a result,this synergistic dual substitution can effectively suppress H2-H3 phase transition and generation of microcracks,thereby ultimately improving the thermodynamic stability of Ni-rich cathode material.Notably,the dual-doped Ni-rich cathode delivers an extremely high capacity retention of 81%after 250 cycles(vs.Li/Li+)in coin-type half cells and 87%after 1000 cycles(vs.graphite/Li^(+))in pouch-type full cells at a high temperature of 55℃.More impressively,the dual-doped sample exhibits excellent thermal stability,which demonstrates a higher thermal runaway temperature and a lower calorific value.The synergetic effects of this dual-substitution strategy pave a new pathway for addressing the critical challenges of Ni-rich cathode at high temperatures,which will significantly advance the high-energy-density and high-safety cathodes to the subsequent commercialization.

关 键 词：Ni-rich cathode Single crystalline Dual-substitution strategy High-temperature cathode Li-ion batteries 

分 类 号：TM912[电气工程—电力电子与电力传动]