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Abstract:
Li-rich layered oxide (LLO) cathode materials with mixedcationicand anionic redox reactions display much higher specific capacitythan other traditional layered oxide materials. However, the practicalspecific capacity of LLO during the first cycle in sulfide all-solid-statelithium-ion batteries (ASSLBs) is extremely low. Herein, the capacitycontribution of each redox reaction in LLO during the first chargingprocess is qualitatively and quantitatively analyzed by comprehensiveelectrochemical and structural measurements. The results demonstratethat the cationic redox of the LiTMO2 (TM = Ni, Co, Mn)phase is almost complete, while the anionic redox of the Li2MnO3 phase is seriously limited due to the sluggish transportkinetics and severe LLO/Li6PS5Cl interface reactionat high voltage. Therefore, the poor intrinsic conductivity and interfacestability during the anionic redox jointly restrict the capacity releaseor delithiation/lithiation degree of LLO during the first cycle insulfide ASSLBs. This study reveals the origin of the seriously limitedanionic redox reaction in LLO, providing valuable guidance for thebulk and interface design of high-energy-density ASSLBs.
