Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution

Tse-Fu Huang; Kuei-Jhong Lin; Ying-Rang Zhuang; Yu-En Sun; Wei-Cheng Lin; Chun-Hao Li; Chien-Cheng Lin; En-Chi Chang; Chih-Li Chang; Yung-Ching Liu; Ling-Yu Hsu; Bing-Heng Li; Wan-Ling Chang; Pimjai Pimbaotham; Cheng-Yun Bai; Wei-Hsiang Huang; Dung Chau Kim Hoang; Khanh Do Gia Huynh; Yi-Chan Huang; Chao-Yan Chung; Mohamed M. Elsenety; Chia-An Chang; Hsin-Ni Huang; Siriporn Jungsuttiwong; Chih-Wen Pao; Hsin-Lung Chen; Tien-Lin Wu; Chia-Chih Chang; Bo-Han Chen; Shang-Da Yang; Kun-Han Lin; Ho-Hsiu Chou

doi:10.1126/sciadv.adx1629

Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution

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Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution

Tse-Fu Huang, Kuei-Jhong Lin, Ying-Rang Zhuang, Yu-En Sun, Wei-Cheng Lin, Chun-Hao Li, Chien-Cheng Lin, En-Chi Chang, Chih-Li Chang, Yung-Ching Liu, …

Science advances, 卷.11(30), 頁.eadx1629

25/07/2025

DOI: https://doi.org/10.1126/sciadv.adx1629

PMID: 40700489

摘要

Chemistry

Physical and Materials Sciences

SciAdv r-articles

Materials Science

The fused sulfone unit has been a key building block for hydrogen evolution photocatalysts for 9 years but still faces the challenge of a poor water/polymer interface due to its rigid structure. This work introduces nonfused, flexible sulfur segments (SSs) into the polymer’s backbone to enhance hydrophilicity and active site access. Unlike rigid, fused sulfone moieties, our flexible SS improves interfacial water contact and charge transport. P-2SO2, with sulfone-functionalized SS, represents a 237% improvement over the control polymer, PBDTTSO. In addition, P-2SO2 demonstrated an outstanding hydrogen evolution rate of 1060.1 micromoles per hour and an apparent quantum yield of 32.4% (460 nanometers). Molecular dynamics simulations indicate SS improves hydrophilicity and water/polymer interface while promoting a hairpin-like conformation that increases intrachain π-π stacking for better charge hopping. Transient absorption spectroscopy shows sulfone-functionalized SS enhances electron transfer to platinum cocatalysts, increases active site density, and reduces exciton migration lengths through stronger polymer/platinum interactions. Adding flexible sulfone segments improves polymer-water interactions and boosts photocatalytic hydrogen evolution efficiency.

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題名: Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution
創作者：: Tse-Fu Huang - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Kuei-Jhong Lin - National Tsing Hua University
Ying-Rang Zhuang - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Yu-En Sun - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Wei-Cheng Lin - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Chun-Hao Li - National Yang Ming Chiao Tung University
Chien-Cheng Lin - National Yang Ming Chiao Tung University
En-Chi Chang - Department of Chemistry, National Tsing Hua University, Hsinchu 300044, Taiwan
Chih-Li Chang - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Yung-Ching Liu - National Tsing Hua University
Ling-Yu Hsu - National Tsing Hua University
Bing-Heng Li - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Wan-Ling Chang - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Pimjai Pimbaotham - National Yang Ming Chiao Tung University
Cheng-Yun Bai - National Yang Ming Chiao Tung University
Wei-Hsiang Huang - National Taiwan University of Science and Technology
Dung Chau Kim Hoang - National Tsing Hua University
Khanh Do Gia Huynh - National Tsing Hua University
Yi-Chan Huang - National Tsing Hua University
Chao-Yan Chung - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Mohamed M. Elsenety - National Tsing Hua University
Chia-An Chang - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Hsin-Ni Huang - National Tsing Hua University
Siriporn Jungsuttiwong - National Synchrotron Radiation Research Center
Chih-Wen Pao - National Synchrotron Radiation Research Center
Hsin-Lung Chen - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Tien-Lin Wu - Department of Chemistry, National Tsing Hua University, Hsinchu 300044, Taiwan. College of Semiconductor Research, National Tsing Hua University, Hsinchu 300044, Taiwan
Chia-Chih Chang - National Yang Ming Chiao Tung University
Bo-Han Chen - National Tsing Hua University
Shang-Da Yang - National Tsing Hua University
Kun-Han Lin - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan
Ho-Hsiu Chou - Department of Chemical Engineering, National Tsing Hua University, Hsinchu 300044, Taiwan. College of Semiconductor Research, National Tsing Hua University, Hsinchu 300044, Taiwan
出版者: American Association for the Advancement of Science
學術資源類型: 期刊文章
出版日期: 25/07/2025
出版資訊: Science advances, 卷.11(30), 頁.eadx1629
語言: 英語

Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution

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