Ni-rich
layered oxide with high reversible capacity, low manufacturing
cost, and high potential is recognized as the best practical cathode
material for high energy density lithium-ion batteries for affordable
electric vehicles. However, they suffer from a poor cycle life owing
to internal microcracks, which have been perceived to be due to anisotropic
volume changes. Herein, the failure mechanism as well as improved
cycle life is demonstrated by a self-assembled molecular monolayer
(SAM) on Ni-rich layered oxide powder with a gas-phase precursor of
octyltrichlorosilane (OTS), enabling mass-scalable manufacturing.
The SAM process with a low heating temperature of 130 °C compared
to the commonly used coating is also suitable to the chemically fragile
Ni-rich layered oxide. Also, a homogeneous angstrom-level OTS coating
is beneficial for preserving the energy density of batteries. In particular,
OTS, with electrolyte-phobic functionality, is very effective for
mitigating the inherent microcrack failure of the particles by reducing
the internal electrolyte decomposition by controlling electrolyte
wetting into secondary particles. Systematic surface analyses of the
cross section of Ni-rich electrode with the OTS coating found greatly
improved particle stability after 100 cycles in comparison with pristine
material.