材料科学
硫化物
电化学
固态
化学工程
电压
纳米技术
电极
工程物理
冶金
物理化学
电气工程
工程类
化学
作者
Gawon Song,Suyeon Lee,Tae-Hun Kim,Min Soo Jung,Kanghyeon Kim,Sung Hee Choi,Seunghyun Lee,Junsung Park,Minseon Lee,Chanhwi Park,Mi‐Sook Kwon,Kyu Tae Lee
标识
DOI:10.1002/aenm.202403374
摘要
Abstract Li‐ and Mn‐rich layered oxides (LMROs) are recognized as promising cathode materials for lithium‐ion batteries (LIBs) due to their high specific capacity and cost efficiency. However, LMROs encounter challenges such as manganese dissolution in electrolytes and the release of oxygen gas from irreversible oxygen redox reactions, leading to structural degradation and voltage decay that reduce energy density. Consequently, recent research has shifted toward employing LMROs in all‐solid‐state batteries (ASSBs), where Mn dissolution is negligible. Herein, nanostructured LMROs demonstrate superior electrochemical compatibility with sulfide‐based solid electrolytes in ASSBs compared to conventional LIBs. Nanostructured LMRO exhibits outstanding capacity retention (97.1% after 1300 cycles at 30 °C) with significantly suppressed voltage decay. Furthermore, the initial electrochemical activation of Li 2 MnO 3 domains within LMRO is explored in terms of the mechano‐electrochemical interactions in the composite cathode. At elevated temperatures, interfacial degradation accelerates due to the chemical oxidation of Li 6 PS 5 Cl solid electrolytes, driven by oxygen released from LMRO. To address this, LMRO surfaces are modified with thioglycolic acid through esterification, suppressing interfacial degradation of Li 6 PS 5 Cl and ensuring stable capacity retention over 500 cycles at 60 °C. These findings underscore the potential of LMRO materials as promising cathode options for ASSBs, surpassing those used in LIBs.
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