Robust Interfacial Effect in Multi-interface Environment through Hybrid Reconstruction Chemistry for Enhanced Energy Storage

Electrochemical-oxidation-driven reconstruction has emerged as an efficient approach for developing advanced materials, but the reconstructed microstructure still faces challenges including inferior conductivity, unsatisfying intrinsic activity, and active-species dissolution. Herein, we present hybrid reconstruction chemistry that synergistically couples electrochemical oxidation with electrochemical polymerization (EOEP) to overcome these constraints. During the EOEP process, the metal hydroxides undergo rapid reconstruction and dynamically couple with polypyrrole (PPy), resulting in an interface-enriched microenvironment. We observe that the interaction between PPy and the reconstructed metal center (i.e., Mn > Ni, Co) is strongly correlated. Theoretical calculation results demonstrate that the strong interaction between Mn sites and PPy breaks the intrinsic limitation of MnO₂, rendering MnO₂ with a metallic property for fast charge transfer and enhancing the ion-adsorption dynamics. Operando Raman measurement confirms the promise of EOEP-treated Mn(OH)₂ (E-MO/PPy) to stably work under a 1.2 V potential window. The tailored E-MO/PPy exhibits a high capacitance of 296 F g^-1 at a large current density of 100 A g^-1. Our strategy presents breakthroughs in upgrading the electrochemical reconstruction technique, which enables both activity and kinetics engineering of electrode materials for better performance in energy-related fields.