Approaching theoretical performances of electrocatalytic hydrogen peroxide generation by cobalt‐nitrogen moieties

Lin, Runjia, Kang, Liqun, Lisowska, Karolina, He, Weiying, Zhao, Siyu, Hayama, Shusaku, Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560, Brett, Dan J. L., Corà, Furio, Parkin, Ivan P. and He, Guanjie 2023. Approaching theoretical performances of electrocatalytic hydrogen peroxide generation by cobalt‐nitrogen moieties. Angewandte Chemie International Edition 62 (21) , e202301433. 10.1002/anie.202301433

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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 H2O2 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 CoN x /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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Additional Information:	License information from Publisher: LICENSE 1: URL: http://creativecommons.org/licenses/by/4.0/
Publisher:	Wiley
ISSN:	1433-7851
Date of First Compliant Deposit:	19 April 2023
Date of Acceptance:	22 March 2023
Last Modified:	05 Jan 2024 08:25
URI:	https://orca.cardiff.ac.uk/id/eprint/158949

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