期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 581, 期 -, 页码 826-835出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2020.07.115
关键词
Visible light; Molecular design; Dye-semiconductor; Anthraquinone; Amines
资金
- National Natural Science Foundation of China [21773173]
- Wuhan University
Through molecular inverse design, researchers have revealed the underlying mechanism of the superior photocatalytic activity of alizarin red S-TiO2 assembly, showing that the substituted -OH groups provide visible light absorption and binding sites, 1,2-DHA plays a major role in photocatalytic activity, and the -SO3 Na+ groups increase the binding strength. The study indicates that this dye-semiconductor assembly can be used for green light-induced selective oxidation reactions.
Dye-semiconductor assemblies are very versatile visible light photocatalysts in terms of tunability by tweaking either dye molecules or semiconductor materials. Here, we adopted a strategy of molecular inverse design of alizarin red S (ARS) to identify the blueprint underlying the superior photocatalytic activity of ARS-TiO2 assembly. We discovered that the substituted -OH groups of anthraquinone provide visible light absorption and binding sites. Importantly, the molecular features of 1,2-dihydroxyanthraquinone (1,2-DHA) contributes mostly to the unique photocatalytic activity after binding with TiO2 with broad visible light absorption which can be maintained at high concentration of amines. Moreover, the electron-withdrawing effect of -SO3 Na+ groups increase the acidities of substituted -OH groups, leading to stronger binding and subsequent higher activity. Ultimately, in situ formed 1,2-DHA-TiO2 assembly can be a powerful photocatalyst for green light-induced selective oxidation of amines into imines with aerial O-2. This work makes evident the promise of molecular design in tailoring dye-semiconductor assemblies for visible light-induced photocatalytic selective chemical transformations. (C) 2020 Elsevier Inc. All rights reserved.
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