Single crystal Ni-rich layered cathodes enabling superior performance in all-solid-state batteries with PEO-based solid electrolytes. Issue 31 (2nd August 2021)

• Record Type: Journal Article
• Authors: Yi, Maoyi; Li, Jie; Fan, Xinming; Bai, Maohui; Zhang, Zhi; Hong, Bo; Zhang, Zhian; Hu, Guorong; Jiang, Huai; Lai, Yanqing
• Is Part Of: Journal of materials chemistry. Volume 9:Issue 31(2021)
• Page Start: 16787
• Page End: 16797
• Publication Date: 2021-08-02
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1ta04476a
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Single-crystal Ni-rich cathodes in ASSBs with PEO-based electrolytes show higher Li + diffusion coefficients, higher specific capacities, and more stable cycling performances relative to polycrystalline cathodes. This is due to the lack of grain boundaries in the structure. Abstract : PEO-based composite electrolytes are very promising in all-solid-state batteries (ASSBs). To achieve ASSBs with high energy density, PEO based composite electrolytes should match high-voltage cathodes, but the stability of the cathode interface is a challenging issue. Herein, we investigate the electrochemical performance of single-crystal LiNi0.6 Mn0.1 Co0.3 O2 (SC-NMC613) in ASSBs with PEO-based electrolytes, and compare the electrochemical performance of SC-NMC613 with conventional polycrystalline LiNi0.6 Mn0.1 Co0.3 O2 (PC-NMC613) systematically. The Li + diffusion coefficient of SC-NMC613 is 2–4 times higher than that of PC-NCM613 in ASSBs. SC-NCM613 shows high initial specific capacity (152 mA h g −1 ) at 0.5C, stable cycling performance (100 cycles, retention of 108.9 mA h g −1 ), and exceptional rate capability even without surface modification, while PC-NCM613 shows low initial specific capacity (137.5 mA h g −1 ) at 0.5C, poor cycling performance (100 cycles, retention of 90.1 mA h g −1 ), and poor rate capability in ASSBs. The severe cycling degradation of PC-NCM613 is mainly attributed to the structural deterioration inside particles and the formation of a rock-salt phase. The SC-NCM613 particles observably alleviate the generation of intergranular cracks and decelerate the formation of the rock-salt phase. SC-NCM cathodes in ASSBs with PEO-based electrolyte are beneficial to the stability of the cathode interface. Therefore, developing single-crystal Ni-rich cathodes represents a promising strategy to achieve ASSBs with both high energy density and power density.