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

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.

Automated summary

Ru-VS2@CC catalysts with Ru clusters anchored to the VS2 surface and VS2 nanosheets embedded in carbon cloth were designed, which exhibited high reactivity and exceptional durability. The Ru clusters were preferentially electro-oxidized to form RuO2 chainmail, providing sufficient catalytic sites and protecting the internal Ru core with VS2 substrates. Theoretical calculations showed that electrons aggregated across the Ru/VS2 interface towards the electro-oxidized Ru clusters, resulting in a positive shift in the Fermi energy level of Ru and optimizing the adsorption capacity of intermediates.