Electronic Structure Reconfiguration of Self-Supported Polyoxometalate-Based Lithium-Ion Battery Anodes for Efficient Lithium Storage

Polyoxometalate (POM)-based materials are considered as promising candidates for lithium-ion batteries (LIBs) due to their stable and well-defined molecular structure and reversible multielectron redox properties. Currently, POM-based electrode materials suffer from high interfacial resistance and low uniformity. Herein, we reported a self-supported POM-based anode material for LIBs by electrodepositing H3PMo12O40 (PMo12) and aniline on carbon cloth (CC) for the first time. The as-prepared polyaniline (PANi)-PMo12/CC composite exhibited an excellent reversible capacity of 1092 mA h g-1 for 200 cycles at 1 A g-1. Such an outstanding performance was attributed to the rapid electron transfer and Li+ diffusion stemming from the exposure of more active sites by the self-supported structure, the strong electrostatic interaction, and electronic structure reconfiguration between the active PMo12 cluster and conductive PANi polymer. This work provides insight into the electronic structure engineering of highly efficient LIB anode materials.