Controlling photocatalytic activity by self-assembly – Tuning perylene bisimide photocatalysts for the hydrogen evolution reaction

McDowall, Daniel, Greeves, Benjamin J., Clowes, Rob, McAulay, Kate, Fuentes-Caparrós, Ana M., Thomson, Lisa, Khunti, Nikul, Cowieson, Nathan, Nolan, Michael C., Wallace, Matthew ORCID: https://orcid.org/0000-0002-5751-1827, Cooper, Andrew I., Draper, Emily R., Cowan, Alexander J. and Adams, Dave J. (2020) Controlling photocatalytic activity by self-assembly – Tuning perylene bisimide photocatalysts for the hydrogen evolution reaction. Advanced Energy Materials, 10 (46). ISSN 1614-6832

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Abstract

Amino acid functionalized perylene bisimides (PBIs) form self-assembled structures in solution, the nature of which depends on the local environment. Using a high-throughput photocatalysis setup, five PBIs are studied for the hydrogen evolution reaction (HER) under a range of conditions (pH and hole scavenger concentration) across 350 experiments to explore the relationship between supramolecular structure and photocatalytic activity. Using small angle X-ray scattering (SAXS), NMR spectroscopy and ultraviolet-visible (UV-vis) absorption spectroscopy, it is shown that photocatalytic activity is determined by the nature of the self-assembled aggregate that is formed, demonstrating the potential of self-assembly to tune activity. There is a clear correlation between the presence of charged flexible cylindrical aggregates and the occurrence of photocatalytic H2 production, with UV–vis spectroscopy indicating that the most active structure type has a distinctive form of π-aggregation which is proposed to enable efficient charge separation across multiple PBI units.

Item Type: Article
Uncontrolled Keywords: hydrogen,organic photocatalysts,self-assembly,solar fuels,renewable energy, sustainability and the environment,materials science(all),sdg 7 - affordable and clean energy ,/dk/atira/pure/subjectarea/asjc/2100/2105
Faculty \ School: Faculty of Science > School of Pharmacy (former - to 2024)
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Depositing User: LivePure Connector
Date Deposited: 07 Nov 2020 01:09
Last Modified: 25 Sep 2024 15:08
URI: https://ueaeprints.uea.ac.uk/id/eprint/77579
DOI: 10.1002/aenm.202002469

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