A simple donor-acceptor linked dyad, 9-mesityl-10-methylacridinium ion (Acr+-Mes) was incorporated into nanosized mesoporous silica-alumina to form a composite, which in acetonitrile is highly dispersed. In this medium, upon visible light irradiation, the formation of an extremely long-lived electron-transfer state (Acr•-Mes•+) was confirmed by EPR and laser flash photolysis spectroscopic methods. The composite of Acr+-Mes-incorporated mesoporous silica-alumina with an added copper complex [(tmpa)CuII](ClO4-)2 (tmpa = tris(2-pyridylmethyl)amine) acts as an efficient and robust photocatalyst for the selective oxygenation of p-xylene by molecular oxygen to produce p-tolualdehyde and hydrogen peroxide. Thus, incorporation of Acr +-Mes into nanosized mesoporous silica-alumina combined with an O2-reduction catalyst ([(tmpa)CuII]2+) provides a promising method in the development of efficient and robust organic photocatalysts for substrate oxygenation by dioxygen, the ultimate environmentally benign oxidant.
CITATION STYLE
Fukuzumi, S., Doi, K., Itoh, A., Suenobu, T., Ohkubo, K., Yamada, Y., & Karlin, K. D. (2012). Formation of a long-lived electron-transfer state in mesoporous silica-alumina composites enhances photocatalytic oxygenation reactivity. Proceedings of the National Academy of Sciences of the United States of America, 109(39), 15572–15577. https://doi.org/10.1073/pnas.1119994109
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