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Substituent effect of conjugated microporous polymers on the photocatalytic hydrogen evolution activity†
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2019-12-30 , DOI: 10.1039/c9ta13212k
Xiaomin Gao 1, 2, 3, 4, 5 , Chang Shu 1, 2, 3, 4, 5 , Chong Zhang 1, 2, 3, 4, 5 , Wenyan Ma 1, 2, 3, 4, 5 , Shi-Bin Ren 6, 7, 8, 9 , Feng Wang 9, 10, 11, 12, 13 , Yu Chen 1, 2, 3, 4, 5 , Jing Hui Zeng 1, 2, 3, 4, 5 , Jia-Xing Jiang 1, 2, 3, 4, 5
Affiliation  

The construction of a donor–acceptor (D–A) organic photocatalyst is a facile approach to improve photocatalytic performances because of the efficient separation of light-generated electrons and holes. The rational design of molecular skeletons and the selection of functional groups are of great importance to an organic photocatalyst with a high photocatalytic activity. Herein, we designed two D–A conjugated microporous polymers (CMPs) with different substituent groups of fluorine atoms and methyl groups on the acceptor unit of dibenzothiophene-dioxide (DBTDO). This study reveals that the introduction of fluorine atoms with strong electron-withdrawing ability onto the acceptor unit can further enhance the electron acceptability of the DBTDO unit, leading to the efficient separation of light-generated electrons and holes, while the introduction of methyl with electron-pushing ability decreases the electron acceptability of the acceptor unit, suppressing the separation of light-generated charge carriers. As a result, the polymer PyDF with fluorine atoms shows an excellent photocatalytic activity compared to PyDM with methyl groups. Under UV/Vis light irradiation, PyDF shows an attractive photocatalytic hydrogen generation rate of 18.93 mmol h−1 g−1, which is much higher than that of PyDM (3.96 mmol h−1 g−1), implying that the functional group acts as a vital role in the catalytic activity of polymer semiconducting photocatalysts.

中文翻译:

共轭微孔聚合物对光催化氢释放活性的取代作用

由于光生电子和空穴的有效分离,构建供体-受体(D-A)有机光催化剂是一种提高光催化性能的简便方法。分子骨架的合理设计和官能团的选择对于具有高光催化活性的有机光催化剂具有重要意义。在这里,我们设计了两种D–A共轭微孔聚合物(CMP),在二苯并噻吩-二氧化物(DBTDO)的受体单元上具有不同的氟原子和甲基取代基。这项研究表明,将具有强吸电子能力的氟原子引入受体单元可以进一步提高DBTDO单元的电子接受度,从而有效分离光生电子和空穴,而引入具有电子推动能力的甲基会降低受体单元的电子接受度,从而抑制了光生电荷载流子的分离。结果,与具有甲基的PyDM相比,具有氟原子的聚合物PyDF显示出优异的光催化活性。在紫外线/可见光照射下,PyDF显示出诱人的光催化氢生成速率为18.93 mmol·h-1 g -1,远高于PyDM(3.96 mmol h -1 g -1),表明官能团在聚合物半导体光催化剂的催化活性中起着至关重要的作用。
更新日期:2020-01-10
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