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dc.contributor.authorWoods, Duncan J.
dc.contributor.authorHillman, Sam A.J.
dc.contributor.authorPearce, Drew
dc.contributor.authorWilbraham, Liam
dc.contributor.authorFlagg, Lucas Q.
dc.contributor.authorDuffy, Warren
dc.contributor.authorMcCulloch, Iain
dc.contributor.authorDurrant, James R.
dc.contributor.authorGuilbert, Anne A.Y.
dc.contributor.authorZwijnenburg, Martijn A.
dc.contributor.authorSprick, Reiner Sebastian
dc.contributor.authorNelson, Jenny
dc.contributor.authorCooper, Andrew I.
dc.identifier.citationWoods, D. J., Hillman, S. A. J., Pearce, D., Wilbraham, L., Flagg, L. Q., Duffy, W., … Cooper, A. I. (2020). Side-chain tuning in conjugated polymer photocatalysts for improved hydrogen production from water. Energy & Environmental Science, 13(6), 1843–1855. doi:10.1039/d0ee01213k
dc.description.abstractStructure-property-activity relationships in solution processable polymer photocatalysts for hydrogen production from water were probed by varying the chemical structure of both the polymer side-chains and the polymer backbone. In both cases, the photocatalytic performance depends strongly on the inclusion of more polar groups, such as dibenzo[b,d]thiophene sulfone backbone units or oligo(ethylene glycol) side-chains. We used optical, spectroscopic, and structural characterisation techniques to understand the different catalytic activities of these systems. We find that although polar groups improve the wettability of the material with water in all cases, backbone and side-chain modifications affect photocatalytic performance in different ways: the inclusion of dibenzo[b,d]thiophene sulfone backbone units improves the thermodynamic driving force for hole transfer to the sacrificial donor, while the inclusion of oligo ethylene glycol side-chains aids the degree of polymer swelling and also extends the electron polaron lifetime. The best performing material, FS-TEG, exhibits a HER of 72.5 μmol h-1 for 25 mg photocatalyst (2.9 mmol g-1 h-1) when dispersed in the presence of a sacrificial donor and illuminated with λ > 420 nm light, corresponding to a hydrogen evolution EQE of 10% at 420 nm. When cast as a thin film, this HER was further boosted to 13.9 mmol g-1 h-1 (3.0 mmol m-2 h-1), which is among the highest rates in this field.
dc.description.sponsorshipAIC, RSS, MAZ, LW, and DW acknowledge the UK Engineering and Physical Sciences Research Council (EPSRC) for funding via grant EP/N004884/1. JN and DP acknowledge funding from the EPSRC via grants EP/P005543/1 and EP/R023581/1. AAYG thanks the EPSRC for award of a research fellowship (EP/P00928X/1). SJH thanks the EPSRC for a Centre for Doctoral Training post-graduate studentship (EP/L016702/1). JN also thanks the European Research Council for support under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 742708) and the Imperial College Research Computing Service for computational resources. JD and IM acknowledge financial support from the KAUST award OSR-2015-CRG4-2572. LQF acknowledges funding from the National Science Foundation (NSF DMR-1607242) and the NSF DMREF (award number 1629369).
dc.publisherRoyal Society of Chemistry (RSC)
dc.rightsThis article is licensed under a Creative Commons Attribution 3.0 Unported License.
dc.titleSide-chain tuning in conjugated polymer photocatalysts for improved hydrogen production from water
dc.contributor.departmentTechnology Transfer
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalEnergy & Environmental Science
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionDepartment of Chemistry and Material Innovation Factory, University of Liverpool Crown Street Liverpool L69 7ZD UK
dc.contributor.institutionDepartment of Physics and Centre for Plastic Electronics, Imperial College London Prince Consort Road London SW7 2AZ UK
dc.contributor.institutionDepartment of Chemistry, University College London 20 Gordon Street London WC1H 0AJ UK
dc.contributor.institutionDepartment of Chemistry, University of Washington Seattle WA 98195-1700 USA
dc.contributor.institutionDepartment of Chemistry and Centre for Plastic Electronics, Imperial College London Exhibition Road London SW7 2AZ UK
kaust.personDuffy, Warren
kaust.personMcCulloch, Iain
kaust.acknowledged.supportUnitResearch Computing

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