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

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.