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使用稳健的双锚定光敏剂实现高效光催化产氢

High-Performance Photocatalytic Hydrogen Generation Using Robust Dianchoring Photosensitizers.

作者信息

Fan Linyu, Wen Yudong, Kwong Wai-Hang, He Xiaojie, Wei Ying, Kwok Yan Yi, Luo Xuwei, Zheng Zhong, Dang Dongfeng, Huang Shuping, Ho Cheuk-Lam

机构信息

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong 310028, PR China.

PolyU Shenzhen Research Institute, Shenzhen, 518055, PR China.

出版信息

ACS Appl Mater Interfaces. 2024 Oct 16;16(41):55437-55451. doi: 10.1021/acsami.4c12018. Epub 2024 Oct 5.

Abstract

A novel series of donor-donor-π-acceptor (D-D-π-A) 9,9'-dihexylfluorene-based dianchoring organic dyes, each featuring distinct bridging electron-donating moieties, have been synthesized and characterized. Their performances in photocatalytic hydrogen evolution (PHE) were evaluated, taking into account of their photophysical and electrochemical attributes. Remarkably, achieved an active and robust H generation system with a turnover number (TON) of up to 17 400 in 126 h, with a production of 1090 μmol (26.3 mL) of hydrogen. The initial turnover frequency (TOF), initial activity (activity), and initial apparent quantum yield (AQY) were 808 h, 505 mmol g h, and 8.65%, respectively, under visible light irradiation in water. This photosensitizer is considered one of the most effective and durable systems for photocatalytic hydrogen production that attached to molecular Pt-TiO, as stated out in the literature using organic dyes under visible light, when compared the TOF and TON values. The experimental results demonstrated that the dianchoring dyes with bridging units could significantly enhance PHE performance, maintaining justifiable durability over prolonged irradiation.

摘要

已经合成并表征了一系列新型的供体-供体-π-受体(D-D-π-A)基于9,9'-二己基芴的双锚定有机染料,每种染料都具有独特的桥连供电子基团。考虑到它们的光物理和电化学特性,评估了它们在光催化析氢(PHE)中的性能。值得注意的是,在126小时内实现了一个活性且稳定的产氢系统,周转数(TON)高达17400,产生了1090μmol(26.3mL)的氢气。在水中可见光照射下,初始周转频率(TOF)、初始活性(activity)和初始表观量子产率(AQY)分别为808 h⁻¹、505 mmol g⁻¹ h⁻¹和8.65%。与文献中使用有机染料在可见光下连接分子Pt-TiO₂时的TOF和TON值相比,这种光敏剂被认为是光催化产氢最有效和最持久的体系之一。实验结果表明,带有桥连单元的双锚定染料可以显著提高PHE性能,并在长时间照射下保持合理的耐久性。

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