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Photocatalytic abstraction of hydrogen atoms from water using hydroxylated graphitic carbon nitride for hydrogenative coupling reactions

Zhang, Dongsheng, Ren, Pengju, Liu, Wuwen, Li, Yaru, Salli, Sofia, Han, Feiyu, Qiao, Wei, Liu, Yu, Fan, Yingzhu, Cui, Yi, Shen, Yanbin, Richards, Emma, Wen, Xiaodong, Rummeli, Mark H., Li, Yongwang, Besenbacher, Flemming, Niemantsverdriet, Hans, Lim, Tingbin and Su, Ren 2022. Photocatalytic abstraction of hydrogen atoms from water using hydroxylated graphitic carbon nitride for hydrogenative coupling reactions. Angewandte Chemie International Edition 134 (24) , e202204256. 10.1002/anie.202204256

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Abstract

Employing pure water, the ultimate green source of hydrogen donor to initiate chemical reactions that involve a hydrogen atom transfer (HAT) step is fascinating but challenging due to its large H−O bond dissociation energy (BDEH-O=5.1 eV). Many approaches have been explored to stimulate water for hydrogenative reactions, but the efficiency and productivity still require significant enhancement. Here, we show that the surface hydroxylated graphitic carbon nitride (gCN−OH) only requires 2.25 eV to activate H−O bonds in water, enabling abstraction of hydrogen atoms via dehydrogenation of pure water into hydrogen peroxide under visible light irradiation. The gCN−OH presents a stable catalytic performance for hydrogenative N−N coupling, pinacol-type coupling and dehalogenative C−C coupling, all with high yield and efficiency, even under solar radiation, featuring extensive impacts in using renewable energy for a cleaner process in dye, electronic, and pharmaceutical industries.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Additional Information: This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Publisher: Wiley
ISSN: 1433-7851
Funders: EPSRC
Date of First Compliant Deposit: 4 May 2022
Date of Acceptance: 25 March 2022
Last Modified: 30 May 2022 10:01
URI: https://orca.cardiff.ac.uk/id/eprint/149522

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