Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution

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-Hua Yu, Yu-Jung Lu, Chi-Chang Hu, Ahmed M. Elewa, Takehisa Mochizuki and Ho-Hsiu Chou ()
Additional contact information
Chih-Li Chang: National Tsing Hua University
Wei-Cheng Lin: National Tsing Hua University
Li-Yu Ting: National Tsing Hua University
Chin-Hsuan Shih: National Cheng Kung University
Shih-Yuan Chen: National Institute of Advanced Industrial Science and Technology
Tse-Fu Huang: National Tsing Hua University
Hiroyuki Tateno: National Institute of Advanced Industrial Science and Technology
Jayachandran Jayakumar: National Tsing Hua University
Wen-Yang Jao: National Tsing Hua University
Chen-Wei Tai: National Tsing Hua University
Che-Yi Chu: National Chung Hsing University
Chin-Wen Chen: National Taipei University of Technology
Chi-Hua Yu: National Cheng Kung University
Yu-Jung Lu: Academia Sinica
Chi-Chang Hu: National Tsing Hua University
Ahmed M. Elewa: National Tsing Hua University
Takehisa Mochizuki: National Institute of Advanced Industrial Science and Technology
Ho-Hsiu Chou: National Tsing Hua University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Photocatalytic water splitting is attracting considerable interest because it enables the conversion of solar energy into hydrogen for use as a zero-emission fuel or chemical feedstock. Herein, we present a universal approach for inserting hydrophilic non-conjugated segments into the main-chain of conjugated polymers to produce a series of discontinuously conjugated polymer photocatalysts. Water can effectively be brought into the interior through these hydrophilic non-conjugated segments, resulting in effective water/polymer interfaces inside the bulk discontinuously conjugated polymers in both thin-film and solution. Discontinuously conjugated polymer with 10 mol% hexaethylene glycol-based hydrophilic segments achieves an apparent quantum yield of 17.82% under 460 nm monochromatic light irradiation in solution and a hydrogen evolution rate of 16.8 mmol m−2 h−1 in thin-film. Molecular dynamics simulations show a trend similar to that in experiments, corroborating that main-chain engineering increases the possibility of a water/polymer interaction. By introducing non-conjugated hydrophilic segments, the effective conjugation length is not altered, allowing discontinuously conjugated polymers to remain efficient photocatalysis.

Date: 2022
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DOI: 10.1038/s41467-022-33211-1

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