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

DOI: 10.1002/aenm.202002469 DOI Help

Authors: Daniel Mcdowall (University of Glasgow) , Benjamin J. Greeves (University of Liverpool) , Rob Clowes (University of Liverpool) , Kate Mcaulay (University of Glasgow) , Ana M. Fuentes‐caparrós (University of Glasgow) , Lisa Thomson (University of Glasgow) , Nikul Khunti (Diamond Light Source) , Nathan Cowieson (Diamond Light Source) , Michael C. Nolan (University of Glasgow; University of Liverpool) , Matthew Wallace (University of East Anglia) , Andrew I. Cooper (University of Liverpool) , Emily R. Draper (University of Glasgow) , Alexander J. Cowan (University of Liverpool) , Dave J. Adams (University of Liverpool)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Advanced Energy Materials , VOL 10

State: Published (Approved)
Published: October 2020
Diamond Proposal Number(s): 20362

Open Access Open Access

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.

Journal Keywords: hydrogen; organic photocatalysts; self‐assembly; solar fuels

Diamond Keywords: Photocatalysis

Subject Areas: Materials, Chemistry, Energy

Instruments: B21-High Throughput SAXS

Added On: 15/12/2020 15:39


Discipline Tags:

Earth Sciences & Environment Sustainable Energy Systems Energy Climate Change Physical Chemistry Catalysis Energy Materials Chemistry Materials Science Organic Chemistry

Technical Tags:

Scattering Small Angle X-ray Scattering (SAXS)