Catalytic Effect of Disordered Ru-O Configurations for Electrochemical Hydrogen Evolution

Abstract

Phase engineering is considered as an effective method for modulating the electronic structure and catalytic activity of catalysts. The disordered conformation of amorphous materials allows flexible reforming of the surface electronic structure, showing their attractiveness as catalysts for hydrogen evolution reaction (HER). Herein, we designed and developed an amorphous ruthenium dioxide (a-RuO₂) catalyst with a disordered Ru-O configuration. The conformational relationship between Ru-O ordering and HER performance is established by combining advanced electron microscopic techniques with detailed electrochemical tests. Specifically, the disordered Ru-O coordination significantly enhanced the HER catalytic activity in both acidic and alkaline media, ultimately leading to HER performance of a-RuO₂ approaching that of commercial Pt/C with higher economics. In addition, a-RuO₂ exhibited excellent stability after 10 h current-time (i-t) testing at 10 mA·cm^-2. Further theoretical simulations showed that the lowered d-band center and optimized electron transport of a-RuO₂ modulated the adsorption strength of the active site to the intermediate reactants, promoting HER kinetics. This work provides a new perspective for exploring highly active HER catalysts through phase engineering.

Keywords

phase engineering / hydrogen evolution reaction / amorphous catalyst / electronic structure

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