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

Abstract

Electrochemical 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 VS₂ surface and the VS₂ nanosheets 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 RuO₂ chainmail, both affording sufficient catalytic sites and protecting the internal Ru core with VS₂ substrates for consistent MSIs. Theoretical calculations elucidate that electrons across the Ru/VS₂ interface 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.