Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 33127912.
- Also identified by DOI 10.1038/s41467-020-19309-4 and PMC identifier 7603490.
- 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
Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M-O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M-O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm<sup>-2</sup> H<sub>2</sub>O<sub>2</sub> current in alkaline and neutral media, respectively) and high H<sub>2</sub>O<sub>2</sub> selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H<sub>2</sub>O<sub>2</sub> production.