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.