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Journal article

Formation of a long-lived electron-transfer state in mesoporous silica-alumina composites enhances photocatalytic oxygenation reactivity

Fukuzumi S, Doi K, Itoh A, Suenobu T, Ohkubo K, Yamada Y, Karlin K...(+7 more)

Proceedings of the National Academy of Sciences, vol. 109, issue 39 (2012) pp. 15572-15577

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Abstract

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 irradn., 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 (tmpa = tris(2-pyridylmethyl)amine) acts as an efficient and robust photocatalyst for the selective oxygenation of p-xylene by mol. oxygen to produce p-tolualdehyde and hydrogen peroxide. Thus, incorporation of Acr+-Mes into nanosized mesoporous silica-alumina combined with an O2-redn. catalyst ((tmpa)CuII2+) provides a promising method in the development of efficient and robust org. photocatalysts for substrate oxygenation by dioxygen, the ultimate environmentally benign oxidant. on SciFinder(R)

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