Zinc-Doped High-Nickel, Low-Cobalt Layered Oxide Cathodes for High-Energy-Density Lithium-Ion Batteries

High-Ni layered oxides with Ni contents greater than 90% are promising cathode candidates for high-energy-density Li-ion batteries. However, drastic electrode–electrolyte reactions and mechanical degradation issues limit their cycle life and practical viability. We demonstrate here that LiNi0.94Co0.04Zn0.02O1.99 (NCZ), obtained by incorporating 2 mol % Zn2+ into an ultrahigh-Ni baseline cathode material LiNi0.94Co0.06O2 (NC), delivers superior cell performance. NCZ retains 74% of the initial capacity after 500 cycles in a full cell assembled with a graphite anode, outperforming NC (62% retention). NCZ also possesses a higher average discharge voltage relative to NC with an outstanding average voltage retention of over 99% after 130 cycles in half cells. Bulk structural investigations unveil that Zn doping promotes a smoother phase transition, suppresses anisotropic lattice distortion, and maintains the mechanical integrity of cathode particles. Furthermore, NCZ shows an enhanced interphase stability after long-term cycling, in contrast to the seriously degraded surface chemistry in NC. This work provides a practically viable approach for designing higher-energy-density high-Ni layered oxide cathodes for lithium-ion batteries.