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Unraveling the Stable Cathode Electrolyte Interface in all Solid-State Thin-Film Battery Operating at 5 V

机译:Unraveling the Stable Cathode Electrolyte Interface in all Solid-State Thin-Film Battery Operating at 5 V

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摘要

Spinel-type LiNi_(0.5)Mn_(1.5)O_4 (LNMO) is one of the most promising 5 V-classcathode materials for Li-ion batteries that can achieve high energy densityand low 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 an 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 indicatesa slight overlithiated layer at the interface prior to cycling, a result thatis consistent with the excess charge capacity measured during the first cycle.Cryogenic electron microscopy further reveals intimate contact betweenLNMO and LiPON without noticeable structure and chemical compositionevolution after extended cycling, demonstrating the superior stability ofLiPON against a high voltage cathode. Consequently, design guidelines areproposed for interface engineering that can accelerate the commercializationof a high voltage cell with solid or liquid electrolytes.

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