Supported photo sensitizers as new efficient materials for gas-phase photo-oxidation

被引:36
作者
Latour, V
Pigot, T
Mocho, P
Blanc, S
Lacombe, S
机构
[1] Fac Sci, CNRS, UMR 5624, Lab Chim Theor & Physicochim Mol, F-64013 Pau, France
[2] CURS, UPPA, Lab Therm, F-64013 Pau, France
关键词
alkysulfide; photo-oxidation; photosensitization; gas-solid reactions; supported photocatalysts;
D O I
10.1016/j.cattod.2005.03.023
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The photosensitised oxidation of dimethyl sulfide in the gas phase was carried out for the first time on original silica materials in a flow reactor and under visible light irradiation. The photocatalysts were prepared either by physisorption of two different photosensitizers, 9,10-dicyanoanthracene or 9,10-anthraquinone on commercial silica beads, or by incorporation of 9,10-dicyanoanthracene in sol-gel monoliths. Oxidation products are mainly sulfoxide, sulfone and disulfide, and it is assumed that singlet oxygen is the most probable reactive oxygen species. These materials display several advantages as they are activated by visible light, and they act as very efficient traps for partially oxidized products. Accordingly, the gas-flow at the outlet of the photocatalytic device is free of any toxic or nauseous product for several days. As soon as products appear in the gas flow, the catalyst is deactivated, but the silica beads can be easily regenerated by mild thermal treatment under controlled conditions. With regard to the photo-oxidative efficiency, our results point out the influence of the properties of the silica support itself, such as transparency, homogeneity and specific surface area. The adsorption capacity of the material is a crucial parameter, as the most DMS adsorbing material is also the most efficient. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:359 / 367
页数:9
相关论文
共 39 条
[1]   Photoxidation of ethylbenzene with air catalyzed by a polymer supported Rose Bengal photosensitizer [J].
Alcántara, R ;
Canoira, L ;
Joao, PG ;
Rodriguez, JG ;
Vázquez, I .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2000, 133 (1-2) :27-32
[2]   Photochemistry of water-soluble quinones.: Production of the hydroxyl radical, singlet oxygen and the superoxide ion [J].
Alegría, AE ;
Ferrer, A ;
Santiago, G ;
Sepúlveda, E ;
Flores, W .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 1999, 127 (1-3) :57-65
[3]  
[Anonymous], 2000, ENTROPIE
[4]   Photosensitizers covalently anchored to the silica surface: Enhanced efficiency of heterogeneous photodechlorination of chlorinated aromatics. [J].
Ayadim, M ;
Soumillion, JP .
TETRAHEDRON LETTERS, 1996, 37 (03) :381-384
[5]   Electron transfer and singlet oxygen mechanisms in the photooxygenation of dibutyl sulfide and thioanisole in MeCN sensitized by N-methylquinolinium tetrafluoborate and 9,10-dicyanoanthracene.: The probable involvement of a thiadioxirane intermediate in electron transfer photooxygenations [J].
Baciocchi, E ;
Del Giacco, T ;
Elisei, F ;
Gerini, MF ;
Guerra, M ;
Lapi, A ;
Liberali, P .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (52) :16444-16454
[6]   OXIDATION OF SULFUR-COMPOUNDS .4. THE PHOTO-OXIDATION OF CH3SH [J].
BALLA, RJ ;
HEICKLEN, J .
JOURNAL OF PHOTOCHEMISTRY, 1985, 29 (3-4) :311-332
[7]  
BENOITMARQUIE F, 1997, THESIS U P SABATIER
[8]   POLYMER-BASED SENSITIZERS FOR PHOTOOXIDATIONS [J].
BLOSSEY, EC ;
NECKERS, DC .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1973, 95 (17) :5820-5822
[9]   THE USE OF INSOLUBLE BENZOYLATED POLYSTYRENE BEADS (POLYMERIC BENZOPHENONE) IN PHOTOCHEMICAL-REACTIONS [J].
BOURDELANDE, JL ;
FONT, J ;
SANCHEZFERRANDO, F .
CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 1983, 61 (05) :1007-1016
[10]   PHOTOCYCLOADDITION OF CYCLOHEXENE AND MALEIC-ANHYDRIDE SENSITIZED BY INSOLUBLE BENZOYLATED POLYSTYRENE [J].
BOURDELANDE, JL ;
FONT, J ;
SANCHEZFERRANDO, F .
TETRAHEDRON LETTERS, 1980, 21 (39) :3805-3808