Authors: 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, Ho-Hsiu Chou
Published: 2022-09-17
DOI: 10.1038/s41467-022-33211-1
Source: Full article
AbstractPhotocatalytic 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.