Many advances made in recent years have highlighted Ni-enriched
nickel, cobalt, manganese (NCM) material as a prospective positive
electrode material for lithium-ion batteries. However, prolonged cycling
is limited by several critical issues, including surface instability,
gas generation, and transitional metal dissolution upon cycling. Here,
we propose a simple interfacial modification approach that uses 1H,1H,2H,2H-perfluorooctyltriethoxysilane (POS) as a coating precursor to improve
surface stability. A one-step thermal heat treatment creates bifunctional
cathode electrolyte interphase (CEI) layers from F- and Si-functionalized
POS, especially at the edge sites of the Ni-enriched NCM cathode,
where serious undesired reactions occur during cycling. The POS-modified
Ni-enriched NCM cathode exhibits improved cycling retention compared
to the unmodified Ni-enriched NCM cathode because parasitic reactions
are well suppressed upon cycling. Systematic analyses show an apparent
inhibition of electrolyte decomposition in the POS-modified Ni-enriched
NCM cathode due to the effective protection of the active edge sites
by the artificial POS-derived CEI layers. The dissolution of metal
components is also greatly decreased because the Si-functional groups
that develop on the POS-derived CEI layers selectively scavenge F– species formed by electrolyte decomposition.