文献类型：期刊文献

英文题名：Synthetic Leaves Based on Crystalline Olefin-Linked Covalent Organic Frameworks for Efficient CO2 Photoreduction with Water

作者：Yang, Na[1];Yan, Wenkai[1];Zhou, Zi-Jian[3];Tian, Chengcheng[2];Zhang, Peng[1];Liu, Honglai[4];Wu, Xin-Ping[3];Xia, Chungu[1];Dai, Sheng[5];Zhu, Xiang[1]

机构：[1]Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China;[2]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Shanghai 200237, Peoples R China;[5]Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA

年份：2024

卷号：24

期号：18

起止页码：5444

外文期刊名：NANO LETTERS

收录：;EI(收录号：20241715981918);WOS:【SCI-EXPANDED(收录号:WOS:001226302000001)】；

基金：X.Z. thanks the financial support from National Natural Science Foundation of China (22078349 and 22005319) and Lanzhou Institute of Chemical Physics (E30159SQ). C.T. was supported by Shanghai Science and Technology Innovation Plan (22DZ1208600), the Innovation Program of Shanghai Municipal Education Commission (2023ZKZD41), and National Natural Science Foundation of China (52170109). X.-P.W. appreciates the support from National Natural Science Foundation of China (52394271). S.D. was supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy.

语种：英文

外文关键词：Olefin-linked covalentorganic frameworks; benzodifurandione-bridgedlinkers; CO2 photoreduction with water; artificial photosynthetic overall reaction; low excitonbinding

摘要：We report, for the first time, a new synthetic strategy for the preparation of crystalline two-dimensional olefin-linked covalent organic frameworks (COFs) based on aldol condensation between benzodifurandione and aromatic aldehydes. Olefin-linked COFs can be facilely crystallized through either a pyridine-promoted solvothermal process or a benzoic anhydride-mediated organic flux synthesis. The resultant COF leaf with high in-plane pi-conjugation exhibits efficient visible-light-driven photoreduction of carbon dioxide (CO2) with water (H2O) in the absence of any photosensitizer, sacrificial agents, or cocatalysts. The production rate of carbon monoxide (CO) reaches as high as 158.1 mu mol g(-1) h(-1) with near 100% CO selectivity, which is accompanied by the oxidation of H2O to oxygen. Both theoretical and experimental results confirm that the key lies in achieving exceptional photoinduced charge separation and low exciton binding. We anticipate that our findings will facilitate new possibilities for the development of semiconducting COFs with structural diversity and functional variability.