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Photocatalytic Partial Water Oxidation Promoted by a Hydrogen Acceptor‐Hydroxyl Mediator Couple
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Photocatalytic Partial Water Oxidation Promoted by a Hydrogen Acceptor‐Hydroxyl Mediator Couple
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Journal Article
Photocatalytic Partial Water Oxidation Promoted by a Hydrogen Acceptor‐Hydroxyl Mediator Couple
2025
Overview
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. Photocatalytic partial water oxidation promoted by a hydrogen acceptor (A) and a hydroxyl mediator (M) couple on CdS nanosheets. While the photogenerated •OH radicals can be stabilized by M to produce ketyl radicals prior to the formation of H2O2, H atoms are transferred to A. This strategy enables a rapid evolution of H2O2 with a high quantum efficiency (16.6%) under visible light irradiation.
Publisher
John Wiley & Sons, Inc,John Wiley and Sons Inc,Wiley
Subject
