Operando Investigation of Zr Doping in NMC811 Cathode for High Energy Density Lithium Ion Batteries

LiNi0.8Mn0.1Co0.1O2 (NMC811) is one of the most promising cathode materials for high energy density Li-ion batteries (LiBs). However, NMC811 suffers from capacity fading during electrochemical cycling because of its structure instability at voltages >4.2 V vs Li|Li⁺ due to the known hexagonal H2→H3 phase transition. Zr doping has proven to be effective in enhancing electrochemical performances of the NMC811. In depth investigations are conducted through operando x-ray diffraction (XRD) and ex situ x-ray absorption spectroscopy (XAS) measurements to mechanistically understand the benefits of Zr-doping in a NMC811 material when doped during the co-precipitation step. Herein, Zr-doping in NMC811 reduces the formation of the detrimental H3 phase and mitigates the transition metal dissolution upon cycling.