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Understanding the failure mechanism towards developing high-voltage single-crystal ni-rich Co-free cathodes

Green Energy & Environment 2024年第6期9卷 1045-1057页

作者： Jixue Shen Bao Zhang Changwang Hao Xiao li Zhiming Xiao Xinyou He Xing Ou Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China Zhejiang Power New Energy Co. Ltd.Zhuji311899China Material Science and Chemistry Engineering College China University of GeosciencesWuhan430074China

Benefited from its high process feasibility and controllable costs,binary-metal layered structured lini_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(liBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible ***,singlecrystal lini_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional lini_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the li/ni antisite defect and dynamic ***,the presence of high li/ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff ***,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal ***,the negative influence of li/ni antisite defect is controllable at low current densities,owing to the attenuated ***,Co-free NM can exhibit better safety performance than that of NCM *** findings are beneficial for understanding the fundamental reaction mechanism of single-crystal ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of liBs with low-cost and high-safety performances.

关键词： li/ni antisite defect Dynamic characteristic High-voltage Single-crystal ni-rich Co-free cathodes lithium-ion batteries

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