Manipulating Li2MnO3-Like Domain Dispersion in Lithium-Rich Layered Oxides Inherited from Precursor

Abstract Leveraging oxygen redox in lithium-rich layered oxides paves the way for increasing the energy density of lithium-ion batteries, whose practical implementation is plagued by poor stability. Although a uniform Li2MnO3-like domain dispersion is suggested to improve cycle stability, the synthesis–structure relationship governing domain formation remains underexplored. Here, we show that Li2MnO3-like domain dispersion is derived by the precursor structure according to the degree of transition-metal separation. Through a comparative investigation of the synthesis mechanism, we reveal the templating effect that more clustered transition-metal oxide precursors lead to more localized Li2MnO3-like ordering in the final cathodes, a tendency also observed with a different lithium source. Furthermore, it is corroborated that cathodes with more dispersed Li2MnO3-like ordering derived from less-ordered precursors exhibit improved electrochemical stability with a mitigated voltage decay. Our findings highlight the significance of precursor design and engineering for structural regulation of high-performance lithium-rich layered oxide cathodes.