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

Title
Formation of a long-lived electron-transfer state in mesoporous silica-alumina composites enhances photocatalytic oxygenation reactivity
Authors
Fukuzumi S.Doi K.Itoh A.Suenobu T.Ohkubo K.Yamada Y.Karlin K.D.
Ewha Authors
Shunichi FukuzumiKenneth D. Karlin
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2012
Journal Title
Proceedings of the National Academy of Sciences of the United States of America
ISSN
0027-8424JCR Link
Citation
vol. 109, no. 39, pp. 15572 - 15577
Indexed
SCI; SCIE; SCOPUS WOS scopus
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 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.
DOI
10.1073/pnas.1119994109
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자연과학대학 > 화학·나노과학전공 > Journal papers
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