Hu Zhicheng, Wang Zhenfeng, Zhang Xi, Tang Haoran, Liu Xiaocheng, Huang Fei, Cao Yong
Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, P. R. China; South China Institute of Collaborative Innovation, Dongguan 523808, PR China.
Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, P. R. China.
iScience. 2019 Mar 29;13:33-42. doi: 10.1016/j.isci.2019.02.007. Epub 2019 Feb 15.
Conjugated polymers are emerging as promising organic photocatalysts for hydrogen evolution from water. However, it is still very challenging for conjugated polymers to realize highly efficient photocatalytic hydrogen evolution. Herein, we demonstrate an efficient strategy of hydrophilic side chain functionalization to boost the hydrogen evolution rates of conjugated polymers. By functionalizing conjugated polymers with hydrophilic oligo (ethylene glycol) monomethyl ether (OEG) side chains, a 90-fold improvement in hydrogen evolution rate has been achieved than that of alkyl-functionalized conjugated polymer. It is found that the OEG side chains interact robustly with Pt co-catalysts, resulting in more efficient charge transfer. Moreover, OEG side chains in conjugated polymers can adsorb H from water, resulting in significantly lowered energy levels on the surfaces of conjugated polymers, which enables cascade energy levels and enhances charge separation and photocatalytic performance. Our results indicate that rational side-chain engineering could facilitate the design of improved organic photocatalysts for hydrogen evolution.
共轭聚合物正成为从水中析氢的有前景的有机光催化剂。然而，共轭聚合物要实现高效光催化析氢仍然极具挑战性。在此，我们展示了一种亲水性侧链功能化的有效策略，以提高共轭聚合物的析氢速率。通过用亲水性低聚（乙二醇）单甲醚（OEG）侧链对共轭聚合物进行功能化，析氢速率比烷基功能化共轭聚合物提高了90倍。研究发现，OEG侧链与铂助催化剂有强烈相互作用，导致电荷转移更高效。此外，共轭聚合物中的OEG侧链可从水中吸附氢，导致共轭聚合物表面的能级显著降低，从而形成级联能级并增强电荷分离和光催化性能。我们的结果表明，合理的侧链工程有助于设计出性能更优的用于析氢的有机光催化剂。
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