New Suggestion of Highly Durable Electrode Design for Ordered Mesoporous Ni–Mn Binary Transition Metal Oxide Anode Material in Lithium‐Ion Batteries

Abstract Anode materials storing large‐scale lithium ions gradually decrease electrochemical performance due to severe volume changes during cycling. Therefore, there is an urgent need to develop anode materials with high electrochemical capacity and durability, without deterioration arising due to the volume changes during the electrochemical processes. To date, mesoporous materials have received attention as anode materials due to their ability to mitigate volume expansion, offer a short pathway for Li + transport, and exhibit anomalous high capacity. However, the nano‐frameworks of transition metal oxide collapse during conversion reactions, demanding an improvement in nano‐framework structure stability. In this study, ordered mesoporous nickel manganese oxide (m‐NMO) is designed as an anode material with a highly durable nanostructure. Interestingly, m‐NMO showed better cycle performance and higher electrochemical capacity than those of nickel oxide and manganese oxide. Operando small‐angle X‐ray scattering and ex situ transmission electron microscopic results confirmed that the binary m‐NMO sustained a highly durable nanostructure upon cycling, unlike the single metal oxide electrodes where the mesostructures collapsed. Ex situ X‐ray absorption spectroscopy proved that nickel and manganese showed different electrochemical reaction voltages, and thus undergoes sequential conversion reactions. As a result, both elements can act as complementary nano‐propping buffers to maintain stable mesostructure.