Photocatalytic partial water oxidation promoted by a hydrogen acceptor-hydroxyl mediator couple

Mai, Yuanqiang, Zhang, Dongsheng, Maliutina, Kristina, Leng, Xueyang, Cai, Nengjun, Li, Jialu, Wang, Chao, Huang, Yu, Zhang, Kai, Zhang, Wujun, Li, Yongwang, Besenbacher, Flemming, Niemantsverdriet, Hans, Liang, Wenting, Shen, Yanbin, Lim, Tingbin, Richards, Emma ORCID: https://orcid.org/0000-0001-6691-2377 and Su, Ren 2024. Photocatalytic partial water oxidation promoted by a hydrogen acceptor-hydroxyl mediator couple. Advanced Science , 2410680. 10.1002/advs.202410680

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Abstract

Hydrogen peroxide (H2O2) is an important chemical in synthetic chemistry with huge demands. Photocatalytic synthesis of H2O2 via oxygen reduction and water oxidation reactions (ORR and WOR) is considered as a promising and desirable solution for on-site applications. However, the efficiency of such a process is low due to the poor solubility of molecular oxygen and the rapid reverse reaction of hydroxyl radicals (•OH) with hydrogen atoms (H). Here, a strategy is proposed to boost the H2O2 evolution via oxidation of water by employing a H acceptor (A, nitrocyclohexane), an •OH mediator (M, dioxane), and a photocatalyst (CdS nanosheets). While •OH radicals are stabilized by dioxane to produce ketyl radicals prior to the formation of H2O2, H atoms are effectively utilized in the generation of cyclohexanone oxime, an important intermediate in the production of Nylon 6. The system displays a rapid kinetic accumulation of H2O2 (0.13 min−1) to a high concentration (6.6 mM). At optimum reaction conditions, a high quantum efficiency (16.6%) and light-to-chemical conversion efficiency (4.9%) can be achieved under 410 nm irradiation.

Item Type:	Article
Date Type:	Published Online
Status:	In Press
Schools:	Chemistry
Publisher:	Wiley
ISSN:	2198-3844
Funders:	EPSRC
Date of First Compliant Deposit:	3 January 2025
Date of Acceptance:	1 November 2024
Last Modified:	30 Jan 2025 15:27
URI:	https://orca.cardiff.ac.uk/id/eprint/174951

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