![]() LiNi 0.8Mn 0.1Co 0.1O 2, NMC811), stand out to compete with the state-of-the-art LIBs in terms of high capacity and high energy density 18, 19, 20, 21. As appealing cathode materials, the layered oxide cathodes, especially the Ni-rich NMC cathodes (e.g. The promise of ASSLBs has stimulated extensive research for the development of ionic conductive SSEs and the successful implementation of high-voltage oxide cathode materials to meet the increasing demands of high-energy-density ASSLBs 6, 7, 8, 9, 10, 11, 12.Īmong various types of SSEs, sulfide SSEs are promising due to their high ionic conductivity up to 10 −2 S cm −1 at 25 ☌, high cation transport number (å 0.9), and good mechanical deformability 13, 14, 15, 16, 17. Solidifying LIBs by substituting the liquid organic electrolytes with solid-state electrolytes (SSEs) to fabricate all-solid-state lithium batteries (ASSLBs) is considered a promising approach due to the significantly improved safety and high theoretical energy density 1, 2, 3, 4, 5. Although conventional non-aqueous liquid electrolyte-based lithium-ion batteries (LIBs) can serve as a power source for many modern applications, there have been gradually raised safety concerns due to the use of flammable organic liquid electrolytes. The development of highly stable energy storage systems is an essential subject to solve the current energy challenges. Indeed, when tested in combination with an indium metal negative electrode and a Li 10GeP 2S 12 solid electrolyte, the gradient oxy-thiophosphate-coated NCM811-based positive electrode enables the delivery of a specific discharge capacity of 128 mAh/g after almost 250 cycles at 0.178 mA/cm 2 and 25 ☌. The tailored surface structure and chemistry of NMC811 hinder the structural degradation associated with the layered-to-spinel transformation in the grain boundaries and effectively stabilize the cathode|solid electrolyte interface during cycling. Via atomic layer deposition of Li 3PO 4 and subsequent in situ formation of a gradient Li 3P 1+xO 4S 4x coating, a precise and conformal covering for NMC811 particles is obtained. To circumvent this issue, here we propose a gradient coating of the NMC811 particles with lithium oxy-thiophosphate (Li 3P 1+xO 4S 4x). High-energy Ni-rich layered oxide cathode materials such as LiNi 0.8Mn 0.1Co 0.1O 2 (NMC811) suffer from detrimental side reactions and interfacial structural instability when coupled with sulfide solid-state electrolytes in all-solid-state lithium-based batteries.
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