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Controlling photocatalytic activity by self‐assembly – tuning perylene bisimide photocatalysts for the hydrogen evolution reaction
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
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
Documents:
aenm.202002469.pdf
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)