Strong Oxide‐Support Interaction over IrO2/V2O5 for Efficient pH‐Universal Water Splitting

Abstract Constructing strong oxide‐support interaction (SOSI) is compelling for modulating the atomic configurations and electronic structures of supported catalysts. Herein, ultrafine iridium oxide nanoclusters (≈1 nm) are anchored on vanadium oxide support (IrO 2 /V 2 O 5 ) via SOSI. The as made catalyst, with a unique distorted IrO 2 structure, is discovered to significantly boost the performance for pH‐universal oxygen evolution reaction (OER). Based on experimental results and theoretical calculations, the distorted IrO 2 active sites with flexible redox states in IrO 2 /V 2 O 5 server as electrophilic centers balance the adsorption of oxo‐intermediates and effectively facilitate the process of OO coupling, eventually propelling the fast turnover of water oxidation. As a result, IrO 2 /V 2 O 5 demonstrates not only ultralow overpotentials at 10 mA cm −2 (266 mV, pH = 0; 329 mV, pH = 7; 283 mV, pH = 14) for OER, but also high‐performance overall water electrolysis over a broad pH range, with a potential of mere 1.50 V (pH = 0), 1.65 V (pH = 7) or 1.49 V (pH = 14) at 10 mA cm −2 . In addition, SOSI can simultaneously secure the distorted active sites and thus remarkably improving the catalytic stability, making it a promising strategy to develop high‐performance catalytic systems.