Accelerated discovery of organic polymer photocatalysts for hydrogen evolution from water through the integration of experiment and theory.



Bai, Yang ORCID: 0000-0002-1643-3770, Wilbraham, Liam, Slater, Benjamin J, Zwijnenburg, Martijn A, Sprick, Reiner Sebastian and Cooper, Andrew I
(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.

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Abstract

Conjugated polymers are an emerging class of photocata-lysts 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 pol-ymers 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 sepa-rate properties can successfully describe up to 68% of the variation in the HER data between the different polymers. The four variables use in the model were the predicted elec-tron affinity, the predicted ionization potential, the optical gap, and the dispersibility of the polymer particles in solu-tion, as measured by optical transmittance.

Item Type: Article
Depositing User: Symplectic Admin
Date Deposited: 28 May 2019 08:51
Last Modified: 10 May 2020 01:30
DOI: 10.1021/jacs.9b03591
URI: http://livrepository.liverpool.ac.uk/id/eprint/3043137

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