Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts.
Nat Commun
; 11(1): 5478, 2020 Oct 30.
Article
en En
| MEDLINE
| ID: mdl-33127912
ABSTRACT
Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H2O2). 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-2 H2O2 current in alkaline and neutral media, respectively) and high H2O2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H2O2 production.
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Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
Nat Commun
Asunto de la revista:
BIOLOGIA
/
CIENCIA
Año:
2020
Tipo del documento:
Article