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Accelerated Discovery of Organic Polymer Photocatalysts for Hydrogen Evolution from Water through the Integration of Experiment and Theory

Bai, Y; Wilbraham, L; Slater, B; Zwijnenburg, MA; Sprick, RS; Cooper, A; (2019) Accelerated Discovery of Organic Polymer Photocatalysts for Hydrogen Evolution from Water through the Integration of Experiment and Theory. Journal of the American Chemical Society , 141 (22) pp. 9063-9071. 10.1021/jacs.9b03591. Green open access

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Abstract

Conjugated polymers are an emerging class of photocatalysts for hydrogen production where the large breadth of potential synthetic diversity presents both an opportunity and a challenge. Here, we integrate robotic experimentation with high-throughput computation to navigate the available structure–property space. A total of 6354 co-polymers was considered computationally, followed by the synthesis and photocatalytic characterization of a sub-library of more than 170 co-polymers. This led to the discovery of new polymers with sacrificial hydrogen evolution rates (HERs) of more than 6 mmol g–1 h–1. The variation in HER across the library does not correlate strongly with any single physical property, but a machine-learning model involving four separate properties can successfully describe up to 68% of the variation in the HER data between the different polymers. The four variables used in the model were the predicted electron affinity, the predicted ionization potential, the optical gap, and the dispersibility of the polymer particles in solution, as measured by optical transmittance.

Type: Article
Title: Accelerated Discovery of Organic Polymer Photocatalysts for Hydrogen Evolution from Water through the Integration of Experiment and Theory
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/jacs.9b03591
Publisher version: https://doi.org/10.1021/jacs.9b03591
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Photocatalysts, Copolymers, Evolution reactions, Materials, Polymers
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/10073729
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