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Selective Oxygen Activation by Integrating Dual Photosensitizers in Conjugated Porous Polymers and Microenvironments Manipulation for High‐Performance Water Purification and H 2 O 2 Production

作者:Danfeng Wang, Wuzi Zhao, Feiyang Tan, Xin Wang, Jingwen Dong, Shiyuan Zhou, Guangfeng Liu, Peiyang Gu · 发表于:Advanced Functional Materials · 年份:2024 · DOI:10.1002/adfm.202419010 · 被引用次数:21 · 研究领域:Advanced Photocatalysis Techniques、Analytical Chemistry and Sensors、Covalent Organic Framework Applications

Abstract Conjugated porous polymers (CPPs) are promising materials for water purification due to their capacity to produce reactive oxygen species (ROS) under visible light. However, insufficient oxygen (O 2 ) adsorption and unselective O 2 activation pathways prevent the efficiency of photodegradation of refractory pollutants. Herein, the strategy of integrating dual photosensitizes into CPPs’ framework in a donor‐π‐acceptor conformation is proposed, combined with microenvironment modulation for regulating exciton dynamic and built‐in electric field, to confer extraordinarily excellent selective and high concentration of singlet oxygen ( 1 O 2 ) production (1.30 × 10 6 µmol g −1 h −1 ), being 10 3 fold of superoxide radical ( · O 2 − ) yield. Consequently, BDP‐Por‐O exhibits unprecedently high efficiency in bisphenol A (BPA) removal, with 10 and 100 ppm BPA degradation in just 2 and 20 min, respectively. Additionally, photocatalytic hydrogen peroxide (H 2 O 2 ) production also shows a satisfactory production rate. Mechanistic investigations using femto‐second transient absorption spectroscopy, Kelvin probe force microscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations reveal the impressive performance is attributed to selective and efficient 1 O 2 generation due to multiple effective O 2 adsorption sites and the access to long‐lived excitons for 1 O 2 permitted by microenvironment optimization. This work provi...