柔性,不熔融的砜功能化聚合物,具有增强的活性位点进入光催化牺牲析氢

IF 12.5 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
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
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引用次数: 0

摘要

9年来,熔融砜单元一直是析氢光催化剂的关键组成部分,但由于其刚性结构,仍然面临着水/聚合物界面不良的挑战。这项工作引入了非熔融,柔性硫段(ss)到聚合物的骨干,以提高亲水性和活性位点的访问。与刚性的熔融砜部分不同,我们的柔性SS改善了界面水接触和电荷传输。砜功能化SS的p - 2so2比对照聚合物PBDTTSO提高了237%。此外,p - 2so2的析氢速率为1060.1微摩尔/小时,表观量子产率为32.4%(460纳米)。分子动力学模拟表明,SS改善了亲水性和水/聚合物界面,同时促进了发夹状构象,增加了链内π-π堆叠,从而更好地实现了电荷跳跃。瞬态吸收光谱表明,砜功能化的SS通过增强聚合物/铂的相互作用,增强了电子向铂共催化剂的转移,增加了活性位点密度,减少了激子迁移长度。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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

Flexible, nonfused sulfone functionalized polymer with enhanced active site access for photocatalytic sacrificial hydrogen evolution
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.
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来源期刊
Science Advances
Science Advances 综合性期刊-综合性期刊
CiteScore
21.40
自引率
1.50%
发文量
1937
审稿时长
29 weeks
期刊介绍: Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.
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