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Structure-activity relationships in well-defined conjugated oligomer photocatalysts for hydrogen production from water

Aitchison, CM; Sachs, M; Little, M; Wilbraham, L; Brownbill, NJ; Kane, C; Blanc, F; ... Cooper, A; + view all (2020) Structure-activity relationships in well-defined conjugated oligomer photocatalysts for hydrogen production from water. Chemical Science 10.1039/d0sc02675a. (In press). Green open access

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Abstract

So far, most organic semiconductor photocatalysts for solar fuels production have been linear polymers or polymeric networks with a broad distribution of molecular weights. Here, we study a series of molecular dibenzo[b,d]thiophene sulfone and fluorene oligomers as well-defined model systems to probe the relationship between photocatalytic activity and structural features such as chain length and planarity. The hydrogen evolution rate was found to vary significantly with bridge head atom, chain length, and backbone twisting. A trimer (S3) of only three repeat units has excellent activity for proton reduction with an EQE of 8.8% at 420 nm, approaching the activity of its polymer analogue and demonstrating that high molar masses are not a prerequisite for good activity. The dynamics of long-lived electrons generated under illumination in the S3 oligomer are also very similar to the corresponding polymer, both under transient and constant irradiation conditions.

Type: Article
Title: Structure-activity relationships in well-defined conjugated oligomer photocatalysts for hydrogen production from water
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d0sc02675a
Publisher version: https://doi.org/10.1039/d0sc02675a
Language: English
Additional information: This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. See here for more information: https://creativecommons.org/licenses/by-nc/3.0/
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10106487
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