  Synthesis of high-performance single crystal LiNi0.8Mn0.1Co0.1O2 (NMC811) in
the absence of molten salt is challenging with no success yet. An innovative
drop-in approach is discovered to synthesize single crystal NMC811 by
controlling the morphology of transition metal hydroxide TM(OH)2 precursors
followed by a simple decomposition step to form transition metal oxide (TMO)
intermediates. Ni redistribution in TMO, as a result of the concurrent
formation of mixed spinel and rock salt phases, helps deagglomerate the later
formed NMC811 clusters of single crystals. As-prepared single crystal NMC811 is
validated in a 2Ah pouch cell demonstrating 1000 stable cycling. The
fundamentally new reaction mechanism of single crystal growth and segregation
without molten salt provides a new direction towards cost-efficient
manufacturing of single crystal NMC811 cathode for advanced lithium-based
batteries.
