Electrochemical Oxidation Encapsulated Ru Clusters Enable Robust Durability for Efficient Oxygen Evolution

Abstract

AbstractElectrochemical oxidization and thermodynamic instability agglomeration are a primary challenge in triggering metal‐support interactions (MSIs) by immobilizing metal atoms on a carrier to achieve efficient oxygen evolution reactions (OER). Herein, Ru clusters anchored to the VS2surface and the VS2nanosheets embedded vertically in carbon cloth (Ru‐VS2@CC) are deliberately designed to realize high reactivity and exceptional durability. In situ Raman spectroscopy reveals that the Ru clusters are preferentially electro‐oxidized to form RuO2chainmail, both affording sufficient catalytic sites and protecting the internal Ru core with VS2substrates for consistent MSIs. Theoretical calculations elucidate that electrons across the Ru/VS2interface aggregate toward the electro‐oxidized Ru clusters, while the electronic coupling of Ru 3p and O 2p orbitals boosts a positive shift in the Fermi energy level of Ru, optimizing the adsorption capacity of the intermediates and diminishing the migration barriers of the rate‐determining steps. Therefore, the Ru‐VS2@CC catalyst demonstrated ultra‐low overpotentials of 245 mV at 50 mA cm−2, while the zinc–air battery maintained a narrow gap (0.62 V) after 470 h of reversible operation. This work has transformed the corrupt into the miraculous and paved a new way for the development of efficient electrocatalysts.