博士生冯依曼论文“Precisely modulating Li2CO3 coverage on Ni-rich cathode for sulfide solid-state lithium battery with unprecedented performance”被Chem接收发表
发布时间:2025-08-28
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All-solid-state lithium batteries (ASSLBs) equipped with Ni-rich layered oxide cathodes (NRLOs) exhibit promising electrochemical performance. However, there is significant controversy regarding the role of carbonate species on the surface of NRLOs. This study explores the impact of surface Li2CO3 on NRLOs in sulfide ASSLBs using CO2 atmosphere treatment to precisely control the Li2CO3 amount. As an electronic insulator, Li2CO3 suppresses space charge effects and interfacial side reactions with the sulfide solid electrolyte, enhancing cycling stability. Surprisingly, the ASSLB with NRLO exposed to CO2 for 20 min demonstrates a capacity of 144 mAh/g at 2 C and maintains the capacity retention of 95.8% after 200 cycles at 0.5 C. However, excessive Li2CO3 impedes ion kinetics, reduces capacity, and promotes CO2 release that degrades electrolyte integrity, leading to rapid failure. The results highlight the critical balance required in surface carbonate regulation for achieving high-energy-density sulfide ASSLBs.