文献类型：期刊文献

英文题名：Nanoscale covalent organic frameworks for enhanced photocatalytic hydrogen production

作者：Zhao, Wei[1,2];Luo, Liang[1,2];Cong, Muyu[3,4];Liu, Xueyan[3,4];Zhang, Zhiyun[3,4];Bahri, Mounib[5];Li, Boyu[1,2];Yang, Jing[1,2];Yu, Miaojie[1,2,3,4];Liu, Lunjie[6];Xia, Yu[6];Browning, Nigel D.[5];Zhu, Wei-Hong[3,4];Zhang, Weiwei[3,4];Cooper, Andrew I.[1,2]

机构：[1]Univ Liverpool, Leverhulme Res Ctr Funct Mat Design, Mat Innovat Factory, Liverpool, England;[2]Univ Liverpool, Dept Chem, Liverpool, England;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai, Peoples R China;[4]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, Shanghai, Peoples R China;[5]Univ Liverpool, Albert Crewe Ctr Electron Microscopy, Liverpool L69 3GL, England;[6]Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

年份：2024

卷号：15

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001285103000019)】；

基金：The authors acknowledge funding from the Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design. The authors thank Dr Yang Bai, Dr Haofan Yang and Chao Li for useful discussions. We thank the Materials Innovation Factory (MIF) team for help with instrument training. We thank the National Natural Science Foundation of China (NSFC, 22375062); Shanghai Municipal Science and Technology Major Project (2018SHZDZX03, 21JC1401700); Shanghai Municipal Science and Technology (20120710200); Shanghai Pilot Program for Basic Research (22TQ1400100-10); the Fundamental Research Funds for the Central Universities; Shanghai Pujiang Program (22PJ1402400); "Chenguang Program" supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission (22CGA32); the Engineering and Physical Sciences Research Council (EPSRC) for financial support under grants EP/N004884/1 and EP/P034497/1. AIC thanks the Royal Society for a Research Professorship (RSRP\S2\232003). W.W.Z. acknowledges the Young Elite Scientists Sponsorship Program by CAST (2023QNRC001) and the Research Center of Analysis and Test of East China University of Science and Technology (ECUST) for assistance with various characterizations. The TEM analysis was performed in the Albert Crewe Centre for Electron Microscopy, a University of Liverpool Shared Research Facility.

语种：英文

摘要：Nanosizing confers unique functions in materials such as graphene and quantum dots. Here, we present two nanoscale-covalent organic frameworks (nano-COFs) that exhibit exceptionally high activity for photocatalytic hydrogen production that results from their size and morphology. Compared to bulk analogues, the downsizing of COFs crystals using surfactants provides greatly improved water dispersibility and light-harvesting properties. One of these nano-COFs shows a hydrogen evolution rate of 392.0 mmol g-1 h-1 (33.3 mu mol h-1), which is one of the highest mass-normalized rates reported for a COF or any other organic photocatalysts. A reverse concentration-dependent photocatalytic phenomenon is observed, whereby a higher photocatalytic activity is found at a lower catalyst concentration. These materials also show a molecule-like excitonic nature, as studied by photoluminescence and transient absorption spectroscopy, which is again a function of their nanoscale dimensions. This charts a new path to highly efficient organic photocatalysts for solar fuel production. Nanosizing covalent organic frameworks using surfactants provides greatly improved water dispersibility and light-harvesting properties, leading to dramatically enhanced photocatalytic hydrogen production performance. Here the authors observe a reverse concentration-dependent photocatalytic phenomeno, whereby a higher photocatalytic activity is found at a lower catalyst concentration.