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

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Bai, Yang and Wilbraham, Liam and Slater, Benjamin J. and Zwijnenburg, Martijn A. and 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, 141 (22). pp. 9063-9071. ISSN 1520-5126 (https://doi.org/10.1021/jacs.9b03591)

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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.

ORCID iDs

Bai, Yang, Wilbraham, Liam, Slater, Benjamin J., Zwijnenburg, Martijn A., Sprick, Reiner Sebastian ORCID logoORCID: https://orcid.org/0000-0002-5389-2706 and Cooper, Andrew I.;
  • Item type:Article
    ID code:74068
    Dates:
    Date
    Event
    5 June 2019
    Published
    10 May 2019
    Published Online
    3 April 2019
    Accepted
    Subjects:Science > Chemistry
    Department:Faculty of Science > Pure and Applied Chemistry
    Depositing user: Pure Administrator
    Date deposited:02 Oct 2020 13:35
    Last modified:18 Dec 2024 16:00
    URI:https://strathprints.strath.ac.uk/id/eprint/74068
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