Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 37481579.
- Also identified by DOI 10.1038/s41467-023-40118-y and PMC identifier 10363113.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Electrocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H<sub>2</sub>O<sub>2</sub> yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e<sup>-</sup> oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H<sub>2</sub>O<sub>2</sub> production. Consequently, the H<sub>2</sub>O<sub>2</sub> yield approaches 30 mol g<sup>-1</sup> h<sup>-1</sup> with a Faradaic efficiency of 80% and excellent durability, yielding a high H<sub>2</sub>O<sub>2</sub> concentration of 7.2 g L<sup>-1</sup>. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e<sup>-</sup> oxygen reduction.