文献类型：期刊文献

英文题名：Rational Design of Covalent Organic Frameworks with Redox-Active Catechol Moieties for High-Performance Overall Photosynthesis of Hydrogen Peroxide

作者：Feng, Shufan[1,2];Cheng, Hao[3];Chen, Feng[1,2];Liu, Xinman[1,2];Wang, Zhiqiang[4,5];Xu, Hangxun[3];Hua, Jianli[1,2]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Joint Int Res Lab Precis Chem, Shanghai 200237, Peoples R China;[3]Univ Sci & Technol China, Dept Polymer Sci & Engn, Key Lab Precis & Intelligent Chem, Hefei 230026, Anhui, Peoples R China;[4]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China

年份：2024

卷号：14

期号：10

起止页码：7736

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20241916054447);WOS:【SCI-EXPANDED(收录号:WOS:001225388500001)】；

基金：For financial support of this research, the authors thank the projects supported by the National Natural Science Foundation of China (22271093, 21788102, 21971064, and 52225307), Shanghai Municipal Science and Technology Major Project (grant no. 2018SHZDZX03), the National Key Research and Development Program of China (2021YFA1500800), the Fundamental Research Funds for the Central Universities (222201717003 and 50321101918001), and the Programme of Introducing Talents of Discipline to Universities (B16017).

语种：英文

外文关键词：redox-active moiety; catechol; covalent organicframeworks; hydrogen peroxide; photocatalysis

摘要：Covalent organic frameworks (COFs) have emerged as promising candidates for solar-driven photosynthesis of hydrogen peroxide (H2O2), yet the development of high-performance COFs tailored for practical applications presents substantial challenges. This research introduces the integration of the redox-active catechol moiety into a series of COFs (TPE-COF-OH, TPB-COF-OH, and TPP-COF-OH), serving as the pivotal active site for photocatalytic oxygen (O-2) reduction to H2O2 through a reversible catechol-quinone interconversion mechanism. This process facilitates the transformation of catechol to o-benzoquinone in the presence of molecular O-2, while photoexcited electrons are utilized to revert o-benzoquinone to catechol, reducing the energy barrier for H2O2 synthesis. Notably, TPB-COF-OH demonstrates an unparalleled H2O2 production rate of 6608 mu mol h(-1) g(-1), outperforming its molecular counterpart, TPB-COF-OMe, which lacks the redox-active catechol unit. Furthermore, TPB-COF-OH achieves a solar-to-chemical conversion efficiency of 0.84%, marking the highest value among COF-based photocatalysts in solar-driven H2O2 production. This investigation not only underscores the critical role of molecular engineering in enhancing COF performance but also broadens the horizon for solar-to-chemical energy conversion technologies.