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



Zhang, Weiwei, Yu, Miaojie, Liu, Tao, Cong, Muyu, Liu, Xueyan, Yang, Haofan, Bai, Yang, Zhu, Qiang, Zhang, Shuo, Gu, Hongxu
et al (show 7 more authors) (2024) Accelerated discovery of molecular nanojunction photocatalysts for hydrogen evolution by using automated screening and flow synthesis. Nature Synthesis, 3 (5). pp. 595-605.

[thumbnail of Accelerated discovery of molecular nanojunction photocatalysts for hydrogen evolution by using automated screening and flow synthesis.pdf] PDF
Accelerated discovery of molecular nanojunction photocatalysts for hydrogen evolution by using automated screening and flow synthesis.pdf - Open Access published version

Download (2MB) | Preview

Abstract

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.

Item Type: Article
Uncontrolled Keywords: 7 Affordable and Clean Energy
Divisions: Faculty of Science and Engineering > School of Physical Sciences
Depositing User: Symplectic Admin
Date Deposited: 22 Mar 2024 15:49
Last Modified: 05 Jun 2024 22:21
DOI: 10.1038/s44160-024-00494-9
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3179816