期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 109, 期 39, 页码 15572-15577出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1119994109
关键词
copper complex catalyst; donor-acceptor dyad; nanosized silica-alumina; p-xylene; photoinduced electron transfer
资金
- Ministry of Education, Culture, Sports, Science and Technology, Japan [20108010, 23750014, 21550061]
- National Institutes of Health [GM28962]
- World Class University [R31-2008-000-10010-0]
- Grants-in-Aid for Scientific Research [23750014, 21550061, 20108010, 24550077] Funding Source: KAKEN
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(center dot)-Mes(center dot+)) 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)Cu-II](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 O-2-reduction catalyst ([(tmpa)Cu-II](2+)) provides a promising method in the development of efficient and robust organic photocatalysts for substrate oxygenation by dioxygen, the ultimate environmentally benign oxidant.
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