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Revisiting the capacity-fading mechanism of P2-type sodium layered oxide cathode materials during high-voltage cycling

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Journal of Energy Chemistry 2022年第6期31卷 16-25,I0002页

作者： Meidan Jiang Guannan Qian Xiao-Zhen Liao Zhouhong Ren Qingyu Dong Dechao Meng Guijia Cui Siqi Yuan Sang-Jun Lee Tian Qin Xi Liu Yanbin Shen Yu-Shi He Liwei Chen Yijin Liu Linsen Li Zi-Feng Ma Department of Chemical Engineering Shanghai Electrochemical Energy Device Research Center(SEED)School of Chemistry and Chemical EngineeringFrontiers Science Center for Transformative MoleculesShanghai Jiao Tong UniversityShanghai 200240China Stanford Synchrotron Radiation Lightsource SLAC National Accelerator LaboratoryMenlo ParkCA 94025United States In-Situ Center for Physical Sciences School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Suzhou Institute of Nanotech and Nanobionics(SINANO) Chinese Academy of SciencesSuzhou 215123JiangsuChina Shanghai Jiao Tong University Sichuan Research Institute Chengdu 610213SichuanChina

P2-type sodium layered oxide cathode (Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)P2-NNMO) has attracted great attention as a promising cathode material for sodium ion batteries because of its high specific capacity. However, this material suffers from a rapid capacity fade during high-voltage cycling. Several mechanisms have been proposed to explain the capacity fade, including intragranular fracture caused by the P2-O2 phase transion, surface structural change, and irreversible lattice oxygen release. Here we systematically investigated the morphological, structural, and chemical changes of P2-NNMO during high-voltage cycling using a variety of characterization techniques. It was found that the lattice distortion and crystal-plane buckling induced by the P2-O2 phase transition slowed down the Na-ion transport in the bulk and hindered the extraction of the Na ions. The sluggish kinetics was the main reason in reducing the accessible capacity while other interfacial degradation mechanisms played minor roles. Our results not only enabled a more complete understanding of the capacity-fading mechanism of P2-NNMO but also revealed the underlying correlations between lattice doping and the moderately improved cycle performance.

关键词： Phase transition Layered cathode Buckling capacity fading mechanism Sodium-ion batteries

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