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Organic Molecule Bifunctionalized Polymeric Carbon Nitride for Enhanced Photocatalytic Hydrogen Peroxide Production

Guiming Ba, Huilin Hu, Xin Chen, Shan Hu, Jinhua Ye, Defa Wang

2023ChemSusChem12 citationsDOI

Abstract

Abstract Modifying the polymeric carbon nitride (CN) with organic molecules is a promising strategy to enhance the photocatalytic activity. However, most previously reported works show that interchain embedding and edge grafting of the organic molecule can hardly be achieved simultaneously. Herein, we successfully synthesized organic molecule bifunctionalized CN (MBCN) through copolymerization of melon and sulfanilamide at a purposely elevated temperature of 550 °C. In MBCN, the edge grafted and interchain embedded benzene rings act as the electron‐donating group and charge‐transfer channel, respectively, rendering efficient photocatalytic H 2 O 2 production. The optimal MBCN exhibits a significantly improved non‐sacrificial photocatalytic H 2 O 2 generation rate (54.0 μmol g −1 h −1 ) from pure water, which is 10.4 times that of pristine CN. Experimental and density functional theory (DFT) calculation results reveal that the enhanced H 2 O 2 production activity of MBCN is mainly attributed to the improved photogenerated charge separation/transfer and decreased formation energy barrier (▵G) from O 2− to the intermediate 1,4‐endoperoxide (⋅OOH). This work suggests that simultaneous formation of electron donating group and charge transfer channel via organic molecule bifunctionalization is a feasible strategy for boosting the photocatalytic activity of CN.

Topics & Concepts

PhotocatalysisMoleculeCarbon nitridePhotochemistryBenzeneMaterials scienceElectron transferElectron acceptorChemical engineeringChemistryCatalysisOrganic chemistryEngineeringAdvanced Photocatalysis TechniquesPerovskite Materials and ApplicationsCovalent Organic Framework Applications
Organic Molecule Bifunctionalized Polymeric Carbon Nitride for Enhanced Photocatalytic Hydrogen Peroxide Production | Litcius