D‐Orbital Manipulated Ru Nanoclusters for High‐Efficiency Overall Water Splitting at Industrial‐Level Current Densities

Abstract Owing to the Pt‐like electrocatalytic capability and moderate price, Ru‐based catalysts are considered as the Pt alternatives for electrochemical water splitting. However, they demonstrate limited catalytic performance under industrial‐level current densities. Herein, a novel electrocatalyst with an extremely low amount (0.85 wt.%) of Ru nanoclusters anchored on Cr‐doped Fe‐metal–organic frameworks (Ru@Cr─FeMOF) through a robust Cr─O─Ru bond is presented. The study unveils that such an architecture facilitates fast electron transfer and manipulates the highest occupied d orbital and d‐band centers of Ru sites, favoring both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalysis. The as‐prepared catalyst performs excellent reaction activity of 21 mV@10 mA cm −2 for HER and 230 mV@50 mA cm −2 for OER in alkaline solution, and realizes excellent water‐splitting performance at industrial‐level current densities (1.72 V@1000 mA cm −2 ), surpassing the state‐of‐the‐art literatures.