Electrochemical Oxidation Encapsulated Ru Clusters Enable Robust Durability for Efficient Oxygen Evolution.
Zhiqian HouChenghao CuiYanan YangTao ZhangPublished in: Small (Weinheim an der Bergstrasse, Germany) (2023)
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 VS 2 surface and the VS 2 nanosheets embedded vertically in carbon cloth (Ru-VS 2 @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 RuO 2 chainmail, both affording sufficient catalytic sites and protecting the internal Ru core with VS 2 substrates for consistent MSIs. Theoretical calculations elucidate that electrons across the Ru/VS 2 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-VS 2 @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.