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Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution

Author

Listed:
  • Michael Sachs

    (Imperial College London)

  • Reiner Sebastian Sprick

    (University of Liverpool
    University of Liverpool)

  • Drew Pearce

    (Imperial College London)

  • Sam A. J. Hillman

    (Imperial College London)

  • Adriano Monti

    (University College London)

  • Anne A. Y. Guilbert

    (Imperial College London)

  • Nick J. Brownbill

    (University of Liverpool)

  • Stoichko Dimitrov

    (Imperial College London
    Swansea University)

  • Xingyuan Shi

    (Imperial College London)

  • Frédéric Blanc

    (University of Liverpool
    University of Liverpool)

  • Martijn A. Zwijnenburg

    (University College London)

  • Jenny Nelson

    (Imperial College London)

  • James R. Durrant

    (Imperial College London)

  • Andrew I. Cooper

    (University of Liverpool
    University of Liverpool)

Abstract

Conjugated polymers have sparked much interest as photocatalysts for hydrogen production. However, beyond basic considerations such as spectral absorption, the factors that dictate their photocatalytic activity are poorly understood. Here we investigate a series of linear conjugated polymers with external quantum efficiencies for hydrogen production between 0.4 and 11.6%. We monitor the generation of the photoactive species from femtoseconds to seconds after light absorption using transient spectroscopy and correlate their yield with the measured photocatalytic activity. Experiments coupled with modeling suggest that the localization of water around the polymer chain due to the incorporation of sulfone groups into an otherwise hydrophobic backbone is crucial for charge generation. Calculations of solution redox potentials and charge transfer free energies demonstrate that electron transfer from the sacrificial donor becomes thermodynamically favored as a result of the more polar local environment, leading to the production of long-lived electrons in these amphiphilic polymers.

Suggested Citation

  • Michael Sachs & Reiner Sebastian Sprick & Drew Pearce & Sam A. J. Hillman & Adriano Monti & Anne A. Y. Guilbert & Nick J. Brownbill & Stoichko Dimitrov & Xingyuan Shi & Frédéric Blanc & Martijn A. Zwi, 2018. "Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-07420-6
    DOI: 10.1038/s41467-018-07420-6
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    Cited by:

    1. Katia Pagano & Jin Gwan Kim & Joel Luke & Ellasia Tan & Katherine Stewart & Igor V. Sazanovich & Gabriel Karras & Hristo Ivov Gonev & Adam V. Marsh & Na Yeong Kim & Sooncheol Kwon & Young Yong Kim & M, 2024. "Slow vibrational relaxation drives ultrafast formation of photoexcited polaron pair states in glycolated conjugated polymers," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Ting He & Wenlong Zhen & Yongzhi Chen & Yuanyuan Guo & Zhuoer Li & Ning Huang & Zhongping Li & Ruoyang Liu & Yuan Liu & Xu Lian & Can Xue & Tze Chien Sum & Wei Chen & Donglin Jiang, 2023. "Integrated interfacial design of covalent organic framework photocatalysts to promote hydrogen evolution from water," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Yan Guo & Qixin Zhou & Jun Nan & Wenxin Shi & Fuyi Cui & Yongfa Zhu, 2022. "Perylenetetracarboxylic acid nanosheets with internal electric fields and anisotropic charge migration for photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Mohamed Hammad Elsayed & Mohamed Abdellah & Ahmed Zaki Alhakemy & Islam M. A. Mekhemer & Ahmed Esmail A. Aboubakr & Bo-Han Chen & Amr Sabbah & Kun-Han Lin & Wen-Sheng Chiu & Sheng-Jie Lin & Che-Yi Chu, 2024. "Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Wei Zhao & Liang Luo & Muyu Cong & Xueyan Liu & Zhiyun Zhang & Mounib Bahri & Boyu Li & Jing Yang & Miaojie Yu & Lunjie Liu & Yu Xia & Nigel D. Browning & Wei-Hong Zhu & Weiwei Zhang & Andrew I. Coope, 2024. "Nanoscale covalent organic frameworks for enhanced photocatalytic hydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Chih-Li Chang & Wei-Cheng Lin & Li-Yu Ting & Chin-Hsuan Shih & Shih-Yuan Chen & Tse-Fu Huang & Hiroyuki Tateno & Jayachandran Jayakumar & Wen-Yang Jao & Chen-Wei Tai & Che-Yi Chu & Chin-Wen Chen & Chi, 2022. "Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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