文献类型：期刊文献

英文题名：Sulfone-containing covalent organic frameworks for photocatalytic hydrogen evolution from water

作者：Wang, Xiaoyan[1,2];Chen, Linjiang[1,2,3,4];Chong, Samantha Y.[1,2];Little, Marc A.[1,2];Wu, Yongzhen[5,6];Zhu, Wei-Hong[5,6];Clowes, Rob[1,2];Yan, Yong[1,2];Zwijnenburg, Martijn A.[7];Sprick, Reiner Sebastian[1,2];Cooper, Andrew I.[1,2,3,4]

机构：[1]Univ Liverpool, Dept Chem, Liverpool, Merseyside, England;[2]Univ Liverpool, Mat Innovat Factory, Liverpool, Merseyside, England;[3]Univ Liverpool, Leverhulme Res Ctr Funct Mat Design, Mat Innovat Factory, Liverpool, Merseyside, England;[4]Univ Liverpool, Dept Chem, Liverpool, Merseyside, England;[5]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai, Peoples R China;[6]East China Univ Sci & Technol, Inst Fine Chem, Shanghai, Peoples R China;[7]UCL, Dept Chem, London, England

年份：2018

卷号：10

期号：12

起止页码：1180

外文期刊名：NATURE CHEMISTRY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000450790300005)】；

基金：The authors acknowledge funding from the Engineering and Physical Sciences Research Council (EPSRC) (EP/N004884/1), the European Union's Seventh Framework Programme through grant agreement nos. 321156 (ERC-AG-PE5-ROBOT) and 692685, and the Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design. X.W. thanks the China Scholarship Council for a PhD studentship. Y.W. and W.-H.Z. acknowledge financial support from the NSFC for Creative Research Groups (21421004) and Key Project (21636002), NSFC/China and a Shanghai Oriental Scholarship. The authors thank M. Bilton for help with HR-TEM, F. McBride for help with AFM, and G.-H. Ning and H. Niu for useful discussions. The authors acknowledge the Diamond Light Source for access to beamlines I19 (MT15777) and I11 (EE12336), the ARCHER UK National Supercomputing Service, access provided via a Programme Grant (EP/N004884/1) and the EPSRC funded UK Materials Chemistry Consortium (EP/L000202/1), and the use of the facilities of the N8 HPC Centre of Excellence, provided and funded by the N8 Research Partnership and EPSRC (EP/K000225/1).

语种：英文

摘要：Nature uses organic molecules for light harvesting and photosynthesis, but most man-made water splitting catalysts are inorganic semiconductors. Organic photocatalysts, while attractive because of their synthetic tunability, tend to have low quantum efficiencies for water splitting. Here we present a crystalline covalent organic framework (COF) based on a benzobis(benzothiophene sulfone) moiety that shows a much higher activity for photochemical hydrogen evolution than its amorphous or semicrystalline counterparts. The COF is stable under long-term visible irradiation and shows steady photochemical hydrogen evolution with a sacrificial electron donor for at least 50 hours. We attribute the high quantum efficiency of fusedsulfone-COF to its crystallinity, its strong visible light absorption, and its wettable, hydrophilic 3.2 nm mesopores. These pores allow the framework to be dye-sensitized, leading to a further 61% enhancement in the hydrogen evolution rate up to 16.3 mmol g(-1) h(-1). The COF also retained its photocatalytic activity when cast as a thin film onto a support.