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

Daniel McDowall, Benjamin J. Greeves, Rob Clowes, Kate McAulay, Ana M. Fuentes-Caparrós, Lisa Thomson, Nikul Khunti, Nathan Cowieson, Michael C. Nolan, Matthew Wallace, Andrew I. Cooper, Emily R. Draper, Alexander J. Cowan*, Dave J. Adams*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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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.
Original languageEnglish
Pages (from-to)1-10
Number of pages10
JournalAdvanced Energy Materials
Early online date26 Oct 2020
DOIs
Publication statusE-pub ahead of print - 26 Oct 2020

Keywords

  • hydrogen
  • organic photocatalysts
  • self‐assembly
  • solar fuels

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