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Approaching Theoretical Performances of Electrocatalytic Hydrogen Peroxide Generation by Cobalt-Nitrogen Moieties.


ABSTRACT: Electrocatalytic oxygen reduction reaction (ORR) has been intensively studied for environmentally benign applications. However, insufficient understanding of ORR 2 e- -pathway mechanism at the atomic level inhibits rational design of catalysts with both high activity and selectivity, causing concerns including catalyst degradation due to Fenton reaction or poor efficiency of H2 O2 electrosynthesis. Herein we show that the generally accepted ORR electrocatalyst design based on a Sabatier volcano plot argument optimises activity but is unable to account for the 2 e- -pathway selectivity. Through electrochemical and operando spectroscopic studies on a series of CoNx /carbon nanotube hybrids, a construction-driven approach based on an extended "dynamic active site saturation" model that aims to create the maximum number of 2 e- ORR sites by directing the secondary ORR electron transfer towards the 2 e- intermediate is proven to be attainable by manipulating O2 hydrogenation kinetics.

SUBMITTER: Lin R 

PROVIDER: S-EPMC10962607 | biostudies-literature | 2023 May

REPOSITORIES: biostudies-literature

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Approaching Theoretical Performances of Electrocatalytic Hydrogen Peroxide Generation by Cobalt-Nitrogen Moieties.

Lin Runjia R   Kang Liqun L   Lisowska Karolina K   He Weiying W   Zhao Siyu S   Hayama Shusaku S   Hutchings Graham J GJ   Brett Dan J L DJL   Corà Furio F   Parkin Ivan P IP   He Guanjie G  

Angewandte Chemie (International ed. in English) 20230418 21


Electrocatalytic oxygen reduction reaction (ORR) has been intensively studied for environmentally benign applications. However, insufficient understanding of ORR 2 e<sup>-</sup> -pathway mechanism at the atomic level inhibits rational design of catalysts with both high activity and selectivity, causing concerns including catalyst degradation due to Fenton reaction or poor efficiency of H<sub>2</sub> O<sub>2</sub> electrosynthesis. Herein we show that the generally accepted ORR electrocatalyst de  ...[more]

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