Litcius/Paper detail

Variation of Chemical Microenvironment of Pores in Hydrazone‐Linked Covalent Organic Frameworks for Photosynthesis of H<sub>2</sub>O<sub>2</sub>

Zhipeng Xie, Xiong Chen, Wenbin Wang, Xiating Ke, Xirui Zhang, Sibo Wang, Xiaofeng Wu, Jimmy C. Yu, Xinchen Wang

2024Angewandte Chemie International Edition108 citationsDOIOpen Access PDF

Abstract

Abstract Photocatalytic synthesis of H 2 O 2 is an advantageous and ecologically sustainable alternative to the conventional anthraquinone process. However, achieving high conversion efficiency without sacrificial agents remains a challenge. In this study, two covalent organic frameworks (COF−O and COF−C) were prepared with identical skeletal structures but with their pore walls anchored to different alkyl chains. They were used to investigate the effect of the chemical microenvironment of pores on photocatalytic H 2 O 2 production. Experimental results reveal a change of hydrophilicity in COF−O, leading to suppressed charge recombination, diminished charge transfer resistance, and accelerated interfacial electron transfer. An apparent quantum yield as high as 10.3 % (λ=420 nm) can be achieved with H 2 O and O 2 through oxygen reduction reaction. This is among the highest ever reported for polymer photocatalysts. This study may provide a novel avenue for optimizing photocatalytic activity and selectivity in H 2 O 2 generation.

Topics & Concepts

PhotocatalysisCovalent bondAlkylChemistryElectron transferChemical engineeringPhotochemistryCovalent organic frameworkAnthraquinonePhotosynthesisHydrazoneElectron transport chainRedoxSelectivityQuantum yieldMaterials scienceOrganic chemistryCatalysisBiochemistryPhysicsQuantum mechanicsEngineeringFluorescenceCovalent Organic Framework ApplicationsAdvanced Photocatalysis TechniquesCatalytic Processes in Materials Science