The strong metal-support interactions induced electrocatalytic three-electron oxygen reduction to hydroxyl radicals for water treatment.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37603765.
- Also identified by DOI 10.1073/pnas.2307989120 and PMC identifier 10466190.
- Licence recorded as CC BY-NC-ND.
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Abstract
As a promising environmental remediation technology, the electro-Fenton (EF) process is mainly limited by the two rate-limiting steps, which are H<sub>2</sub>O<sub>2</sub> generation and activation. The electrocatalytic three-electron oxygen reduction reaction (3e<sup>-</sup> ORR) can directly activate oxygen to hydroxyl radicals (•OH), which is expected to break through the rate-limiting steps of the EF process. However, limited success has been achieved in the design of 3e<sup>-</sup> ORR electrocatalysts. Herein, we propose Cu/CoSe<sub>2</sub>/C with the strong metal-support interactions to enhance the 3e<sup>-</sup> ORR process, exhibiting remarkable reactivity and stability for •OH generation. Both experiment and DFT calculation results reveal that CoSe<sub>2</sub> is conducive to the generation of H<sub>2</sub>O<sub>2</sub>. Meanwhile, the metallic Cu can enhance the adsorption strength of *H<sub>2</sub>O<sub>2</sub> intermediates and thus promotes the one-electron reduction to •OH. The Cu/CoSe<sub>2</sub>/C catalyst exhibits the electron-transfer number close to 3.0 during the ORR process, and exhibits the outstanding •OH generation performance, achieving a higher apparent rate constant (6.0 times faster) toward ciprofloxacin compared with its analogy without the SMSI effect. Our work represents that the SMSI effect endows Cu/CoSe<sub>2</sub>/C high activity and selectivity for •OH generation, providing a unique perspective for the design of a high-efficiency 3e<sup>-</sup> ORR catalyst.