光催化
部分
光化学
噻吩
三苯胺
烷基
电子供体
接受者
化学
连接器
氢
量子产额
制氢
材料科学
催化作用
有机化学
物理
量子力学
计算机科学
荧光
操作系统
凝聚态物理
作者
Yan-Yi Kwok,Po‐Yu Ho,Ying Wei,Zhong Zheng,Sze Chun Yiu,Cheuk Lam Ho,Shuping Huang
标识
DOI:10.1021/acs.chemmater.2c00556
摘要
Six donor–donor−π–acceptor (D–D−π–A) triphenylamine-based starburst organic dyes with different electron-donating moieties and thiophene-based π-linkers were synthesized and characterized. Their photophysical and electrochemical properties, together with their photocatalytic hydrogen evolution performance as photosensitizers (PSs), were investigated. Distinctive and prolonged hydrogen evolution performances of these PSs under visible-light irradiation from water in their platinized TiO2 composites were demonstrated: a turnover number (TON) of up to 24 900 (252 h) with 1560 μmol (37.6 mL) hydrogen produced, an initial turnover frequency (TOFi) of 1130 h–1, initial activity (Activityi) of 705 mmol g–1 h–1, and initial apparent quantum yield (AQYi) of 12.1%. To the best of our knowledge, according to the TOF and TON values, the designed PS system is one of the most efficient and robust photocatalytic H2 generation systems adopting a TiO2-anchoring molecular PS in the literature. The results showed that the starburst triarylamine donor moiety with phenothiazine functionality and the alkyl chain on the thiophene π-linker could boost the performance and longevity of the photocatalytic system, providing a powerful strategy for the development of starburst-based highly efficient and robust D–D−π–A organic photosensitizers in the future.
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