文献类型：期刊文献

英文题名：Accelerated discovery of molecular nanojunction photocatalysts for hydrogen evolution by using automated screening and flow synthesis

作者：Zhang, Weiwei[1,2];Yu, Miaojie[1,2,3,4];Liu, Tao[3,4];Cong, Muyu[1,2];Liu, Xueyan[1,2];Yang, Haofan[3,4];Bai, Yang[3,4];Zhu, Qiang[3,4];Zhang, Shuo[1,2];Gu, Hongxu[1,2];Wu, Xiaofeng[1,2,3,4];Zhang, Zhiyun[1,2];Wu, Yongzhen[1,2];Tian, He[1,2];Li, Xiaobo[5];Zhu, Wei-Hong[1,2];Cooper, Andrew I.[1,2,3,4]

机构：[1]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn, Key Lab Adv Mat,Feringa Nobel Prize Scientist Join, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn,Inst Fine, Shanghai, Peoples R China;[3]Univ Liverpool, Leverhulme Res Ctr Funct Mat Design, Mat Innovat Factory, Liverpool, England;[4]Univ Liverpool, Dept Chem, Liverpool, England;[5]Zhejiang Normal Univ, Inst Phys Chem, Zhejiang Key Lab React Chem Solid Surfaces, Key Lab,Minist Educ Adv Catalysis Mat, Jinhua 321004, Peoples R China

年份：2024

卷号：3

期号：5

起止页码：595

外文期刊名：NATURE SYNTHESIS

收录：WOS:【ESCI(收录号:WOS:001181025700001)】；

基金：We thank the National Natural Science Foundation of China (NSFC, 22338006, 22372151, 9235630033 and 22375062); Shanghai Municipal Science and Technology Major Project (2018SHZDZX03, 21JC1401700); the Shanghai Pilot Program for Basic Research (22TQ1400100-10); Shanghai Municipal Science and Technology (20120710200); Fundamental Research Funds for the Central Universities; the Shanghai Pujiang Program (22PJ1402400); the 'Chenguang Program' supported by the Shanghai Education Development Foundation and the 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; and the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang (2022R01007). 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 and C. Zhao from ECUST for useful discussion on theoretical calculations. M.Y. acknowledges the China Scholarship Council (CSC) for financial support. A.I.C. thanks the Royal Society for a Research Professorship (RSRP\S2\232003).

语种：英文

摘要：Discovering and optimizing multicomponent organic semiconductors is typically a laborious process. High-throughput experimentation can accelerate this, but the results of small-scale screening trials are not always transferable to bulk materials production. Here we report the accelerated discovery of molecular nanojunction photocatalysts based on a combinatorial donor-acceptor molecular library assisted by high-throughput automated screening. The knowledge gained from this high-throughput batch screening is then transferred to a scaled-up, flow-based synthesis process. The scaled-up molecular nanojunction MTPA-CA:CNP147 (3-(4-(bis(4-methoxyphenyl)amino)phenyl)-2-cyanoacrylic acid:2,6-bis(4-cyanophenyl)-4-(4 '-fluoro-[1,1 '-biphenyl]-4-yl)pyridine-3,5-dicarbonitrile) exhibits a sacrificial hydrogen evolution rate of 330.3 mmol h-1 g-1 with an external quantum efficiency of 80.3% at 350 nm, which are among the highest reported for an organic photocatalyst. A one-dimensional nanofibre architecture is identified for this molecular nanojunction, which exhibits efficient charge separation. Electronic structure-property correlations across the photocatalyst library show that a moderate binding energy between the donor and the acceptor molecules is a potential factor for efficient molecular nanojunction formation. An efficient molecular nanojunction photocatalyst for hydrogen evolution is identified from a combinatorial molecular library, assisted by a materials acceleration platform, which is then scaled-up to the litre scale using flow synthesis.