Tailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi_(0.5)Mn_(1.5)O_4 Spinel Cathode Materials

Sun Huabin; Hu Anyang; Spence StephanieKuai ChunguangHou DongMu LinqinLiu JueLi LuxiSun ChengjunSainio SamiNordlund DennisLuo WeiHuang YunhuiLin Feng

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Tailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi_(0.5)Mn_(1.5)O_4 Spinel Cathode Materials

机译：Tailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi_(0.5)Mn_(1.5)O_4 Spinel Cathode Materials

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In the spinel oxide cathode family, LiNi0.5Mn1.5O4 (LNMO) shows a high operating voltage (approximate to 4.7 V vs Li/Li+) and excellent Li-ion mobility with stable 3D conducting channels. Ni/Mn cation disordered and ordered phases usually coexist in LNMO materials, and they have distinct structural and electrochemical properties, resulting in different battery performances for LNMO materials with different phase compositions. Identifying the correlation between phase compositions and electrochemical properties is of significance to the improvement of battery performance and understanding of degradation mechanisms. Herein, the disordered/ordered phase compositions in LNMO materials are tailored by post-annealing strategies and their impacts on electrochemical performance and degradation mechanisms from the surface to the bulk are systematically investigated. The ordered phase increases rapidly as Mn3+ is oxidized to Mn4+ through a post-annealing process. LNMO with an intermediate fraction of disordered and ordered phases gives rise to improved cycling stability. This article further reports that a high ordered phase fraction can preferentially protect Ni from dissolution during cycling. However, these results suggest that the transition metal dissolution and surface structural change of LNMO do not exhibit a direct correlation with cycling stability. These results indicate the capacity fading mainly correlates with the bulk structural distortion, leading to decreased Li-ion kinetics.

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《Advanced functional materials》 |2022年第21期|2112279.1-2112279.10|共10页
作者
Sun Huabin; Hu Anyang; Spence StephanieKuai ChunguangHou DongMu LinqinLiu JueLi LuxiSun ChengjunSainio SamiNordlund DennisLuo WeiHuang YunhuiLin Feng;
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作者单位

Virginia Tech, Dept Chem, Blacksburg, VA 24061 USA|Tongji Univ, Sch Mat Sci & Engn, Inst New Energy Vehicles, Shanghai 201804, Peoples R China;

Virginia Tech, Dept Chem, Blacksburg, VA 24061 USA;

Oak Ridge Natl Lab, Neutron Scattering Div, POB 2009, Oak Ridge, TN 37831 USAArgonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 60439 USASLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA|Univ Oulu, Fac Informat Technol & Elect Engn, Microelect Res Unit, POB 4500, Oulu 90570, FinlandSLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USATongji Univ, Sch Mat Sci & Engn, Inst New Energy Vehicles, Shanghai 201804, Peoples R China;

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正文语种英语
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cycle life; disorder-to-order transition; fading mechanism; metal dissolution; spinel cathodes;

Tailoring Disordered/Ordered Phases to Revisit the Degradation Mechanism of High-Voltage LiNi_(0.5)Mn_(1.5)O_4 Spinel Cathode Materials

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