Decoupling the Effects of Ruthenium Sites and Oxygen Vacancies on the Mechanism Regulation of Acidic Water Oxidation.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41489370.
- Also identified by DOI 10.1021/acsnano.5c21185.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Precise regulation of the oxygen evolution reaction (OER) pathway to a more favorable lattice oxygen mechanism (LOM) is essential for achieving high-performance acidic OER electrocatalysts. Although cation doping and oxygen vacancy (O<sub>v</sub>) engineering are fundamental strategies, their individual contributions to activating the LOM mechanism remain unclear. Herein, we report a Ru-doped Co<sub>3</sub>O<sub>4</sub> catalyst enriched with O<sub>v</sub> (Ru-Co<sub>3</sub>O<sub>4-<i>x</i></sub>) as the model system to decouple these effects. Combined experimental characterizations and density functional theory (DFT) calculations reveal that O<sub>v</sub> can exclusively promote the LOM mechanism, while Ru dopants minimally alter the catalytic pathway. The incorporation of Ru enables the electron redistribution within the lattice of Ru-Co<sub>3</sub>O<sub>4-<i>x</i></sub>, enhancing the adsorption of key reaction intermediates, thereby lowering the reaction energy barriers. The electron localization at Ru sites is also responsible for improved stability in harsh conditions. As a result, Ru-Co<sub>3</sub>O<sub>4-<i>x</i></sub> delivers a relatively low overpotential of 198 mV at 10 mA cm<sup>-2</sup> and is capable of operating stably for more than 220 h. Our findings not only underscore the synergistic effects of Ru doping and O<sub>v</sub> incorporation in enhancing acidic OER performance but also decouple the effects of Ru sites and oxygen vacancies on the mechanism regulation, providing valuable guidance for designing and optimizing high-performance acidic OER catalysts.