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Spinel-type LiNi0.5Mn1.5O4 (LNMO) is one of the most promising 5 V-classcathode materials for Li-ion batteries that can achieve high energy density andlow production costs. However, in liquid electrolyte cells, the high voltagecauses continuous cell degradation through the oxidative decomposition ofcarbonate-based liquid electrolytes. In contrast, some solid-state electrolyteshave a wide electrochemical stability range and can withstand the requiredoxidative potential. In this work, a thin-film battery consisting of a LNMOcathode with a solid lithium phosphorus oxynitride (LiPON) electrolyte istested and their interface before and after cycling is characterized. With Limetal as the anode, this system can deliver stable performance for 600 cycleswith an average Coulombic efficiency > 99%. Neutron depth profiling indicates aslight overlithiated layer at the interface prior to cycling; a result that isconsistent with the excess charge capacity measured during the first cycle.Cryogenic electron microscopy further reveals intimate contact between LNMO andLiPON without noticeable structure and chemical composition evolution afterextended cycling, demonstrating the superior stability of LiPON against a highvoltage cathode. Consequently, we propose design guidelines for interfaceengineering that could accelerate the commercialization of a high voltage cellwith solid or liquid electrolytes.

Unraveling the stable cathode electrolyte interface in all solid-state thin-film battery operating at 5V