Controlling photocatalytic activity by self-assembly – tuning perylene bisimide photocatalysts for the Hydrogen Evolution Reaction

McDowall, D. et al. (2020) Controlling photocatalytic activity by self-assembly – tuning perylene bisimide photocatalysts for the Hydrogen Evolution Reaction. Advanced Energy Materials, 10(46), 2002469. (doi: 10.1002/aenm.202002469)

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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:Articles
Additional Information:Financial support for this work is from the EPSRC EP/P034497/1, EP/L021978/1, L/021978/2 and Leverhulme Trust RPG‐2018‐013.
Glasgow Author(s) Enlighten ID:Nolan, Michael and Thomson, Miss Lisa and Adams, Dave and McDowall, Mr Daniel and Draper, Emily and McAulay, Dr Kate and Fuentes Caparros, Miss Ana Maria
Authors: McDowall, D., Greeves, B. J., Clowes, R., McAulay, K., Fuentes‐Caparrós, A. M., Thomson, L., Khunti, N., Cowieson, N., Nolan, M. C., Wallace, M., Cooper, A., Draper, E. R., Cowan, A. R.., and Adams, D. J.
College/School:College of Science and Engineering
College of Science and Engineering > School of Chemistry
Journal Name:Advanced Energy Materials
ISSN (Online):1614-6840
Published Online:26 October 2020
Copyright Holders:Copyright © 2020 The Authors
First Published:First published in Advanced Energy Materials 10(46): 2002469
Publisher Policy:Reproduced under a Creative Commons Licence

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
174004Multicomponent Supramolecular HydrogelsDave AdamsEngineering and Physical Sciences Research Council (EPSRC)EP/L021978/2Chemistry