High Energy Density Single-Crystal NMC/Li(6)PS(5)Cl Cathodes for All-Solid-State Lithium-Metal Batteries

[Image: see text] To match the high capacity of metallic anodes, all-solid-state batteries require high energy density, long-lasting composite cathodes such as Ni–Mn–Co (NMC)-based lithium oxides mixed with a solid-state electrolyte (SSE). However in practice, cathode capacity typically fades due to NMC cracking and increasing NMC/SSE interface debonding because of NMC pulverization, which is only partially mitigated by the application of a high cell pressure during cycling. Using smart processing protocols, we report a single-crystal particulate LiNi(0.83)Mn(0.06)Co(0.11)O(2) and Li(6)PS(5)Cl SSE composite cathode with outstanding discharge capacity of 210 mA h g(–1) at 30 °C. A first cycle coulombic efficiency of >85, and >99% thereafter, was achieved despite a 5.5% volume change during cycling. A near-practical discharge capacity at a high areal capacity of 8.7 mA h cm(–2) was obtained using an asymmetric anode/cathode cycling pressure of only 2.5 MPa/0.2 MPa.