Unveiling the correlation between structural alterations and enhanced high-voltage cyclability in Na-deficient P3-type layered cathode materials via Li incorporation  

作　　者：Xiaoxia Yang Suning Wang Hang Li Jochi Tseng Zhonghua Wu Sylvio Indris Helmut Ehrenberg Xiaodong Guo Weibo Hua 

机构地区：[1]School of Chemical Engineering and Technology,Xi'an Jiaotong University,Xi'an,China [2]School of Chemical Engineering,Sichuan University,Chengdu,China [3]Institute for Applied Materials(IAM),Karlsruhe Institute of Technology(KIT),Eggenstein‐Leopoldshafen,Germany [4]Diffraction and Scattering Division,Japan Synchrotron Radiation Research Institute(JASRI),Kouto,Sayo‐cho,Sayo‐gun,Hyogo,Japan [5]Beijing Synchrotron Radiation Facility,Institute of High Energy Physics,Chinese Academy of Sciences,Beijing,China

出　　处：《Electron》2024年第1期164-176,共13页电子（英文）

基　　金：Distinguished Young Foundation of Sichuan Province,Grant/Award Number:2020JDJQ0027;National Natural Science Foundation of China,Grant/Award Numbers:22108218,20A20145,21878195;German Research Foundation,Grant/Award Number:390874152;“Young Talent Support Plan”of Xi'an Jiaotong University,Grant/Award Number:HG6J016;Qinchuangyuan Innovative Talent Project,Grant/Award Number:QCYRCXM-2022-137。

摘　　要：With exceptional capacity during high-voltage cycling,P3-type Nadeficient layered oxide cathodes have captured substantial attention.Nevertheless,they are plagued by severe capacity degradation over cycling.In this study,tuning and optimizing the phase composition in layered oxides through Li incorporation are proposed to enhance the high-voltage stability.The structural dependence of layered Na_(2/3)LixNi_(0.25)Mn_(0.75)O_(2)þδoxides on the lithium content(0.0≤x≤1.0)offered during synthesis is investigated systematically on an atomic scale.Surprisingly,increasing the Li content triggers the formation of mixed P2/O3-type or P3/P2/O3-type layered phases.As the voltage window is 1.5-4.5 V,P3-type Na2/3Ni_(0.25)Mn_(0.75)O_(2)(NL0.0NMO,R3m)material exhibits a sequence of phase transformations throughout the process of(de)sodiation,that is,O3⇌P3⇌O30⇌O3″.Such complicated phase transitions can be effectively suppressed in the Na2/3Li_(0.7)Ni_(0.25)Mn_(0.75)O_(2.4)(NL_(0.7)NMO)oxide with P2/P3/O3-type mixed phases.Consequently,cathodes made of NL0.7NMO exhibit a substantially enhanced cyclic performance at high voltages compared to that of the P3-type layered NL0.0NMO cathode.Specifically,NL0.7NMO demonstrates an outstanding capacity retention of 98%after 10 cycles at 1 C within 1.5-4.5 V,much higher than that of NL0.0NMO(83%).This work delves into the intricate realm of bolstering the high-voltage durability of layered oxide cathodes,paving the way for advanced sodium-ion battery technologies.

关 键 词：high-voltage cycling Li incorporation phase transition sodium ion batteries triphasic composites 

分 类 号：TB381[一般工业技术—材料科学与工程]