In situ UV-vis and EPR study on the formation of hydroperoxide species during direct gas phase propylene epoxidation over Au/Ti-SiO2 catalyst

被引:138
作者
Chowdhury, Biswajit [1 ]
Bravo-Suarez, Juan J. [1 ]
Mimura, Naoki [1 ]
Lu, Jiqing [1 ]
Bando, Kyoko K. [1 ]
Tsubota, Susumu [1 ]
Haruta, Masatake [1 ]
机构
[1] Natl Inst Adv Ind Sci & Technol, Res Inst Innovat Sustainable Chem, Tsukuba, Ibaraki 3058569, Japan
关键词
D O I
10.1021/jp066008y
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In recent years, there have been great experimental and theoretical advances in the understanding of the epoxidation of propylene by O-2 and H-2 over Au supported on titanium-containing oxidic supports; however, thus far spectroscopic evidence of reacting species for proposed mechanisms has been lacking. Hydroperoxide species have been postulated as an intermediate responsible for the epoxidation of propylene with O-2 and H-2. In order to obtain direct evidence for the different type of active oxygen species, in situ UV-vis and EPR measurements were carried out during the epoxidation of propylene with O-2 and H-2 over a Au/Ti-SiO2 (Ti/Si = 3:100) catalyst. It was determined that the adsorbed species of oxygen (O-2(-)) resided on Au, more likely at a perimeter site, and it led to the formation of titanium hydroperoxo species. These results support the possible mechanism of formation of these hydroperoxo species via H2O2 produced from O-2 and H-2 adsorbed on the Au surfaces.
引用
收藏
页码:22995 / 22999
页数:5
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共 47 条
  • [31] Direct production of hydrogen peroxide from H2 and O2 over highly dispersed Au catalysts
    Okumura, M
    Kitagawa, Y
    Yamagcuhi, K
    Akita, T
    Tsubota, S
    Haruta, M
    [J]. CHEMISTRY LETTERS, 2003, 32 (09) : 822 - 823
  • [32] EPR study of CO and O2 interaction with supported Au catalysts
    Okumura, M
    Coronado, JM
    Soria, J
    Haruta, M
    Conesa, JC
    [J]. JOURNAL OF CATALYSIS, 2001, 203 (01) : 168 - 174
  • [33] HYDROGEN-PEROXIDE SYNTHESIS OVER METALLIC CATALYSTS
    OLIVERA, PP
    PATRITO, EM
    SELLERS, H
    [J]. SURFACE SCIENCE, 1994, 313 (1-2) : 25 - 40
  • [34] Absolute determination of reaction mechanisms by in situ measurements of reaction intermediates
    Oyama, ST
    Li, W
    [J]. TOPICS IN CATALYSIS, 1999, 8 (1-2) : 75 - 80
  • [35] Epoxidation of propylene over gold catalysts supported on non-porous silica
    Qi, CX
    Akita, T
    Okumura, M
    Haruta, M
    [J]. APPLIED CATALYSIS A-GENERAL, 2001, 218 (1-2) : 81 - 89
  • [36] Active sites and reactive intermediates in titanium silicate molecular sieves
    Ratnasamy, P
    Srinivas, D
    Knözinger, H
    [J]. ADVANCES IN CATALYSIS, VOL 48, 2004, 48 : 1 - 169
  • [37] Distinguishing between reaction intermediates and spectators: A kinetic study of acetone oxidation using ozone on a silica-supported manganese oxide catalyst
    Reed, C
    Xi, Y
    Oyama, ST
    [J]. JOURNAL OF CATALYSIS, 2005, 235 (02) : 378 - 392
  • [38] Reactive oxygen species in epoxidation reactions over titanosilicate molecular sieves
    Shetti, VN
    Manikandan, P
    Srinivas, D
    Ratnasamy, P
    [J]. JOURNAL OF CATALYSIS, 2003, 216 (1-2) : 461 - 467
  • [39] A three-dimensional mesoporous titanosilicate support for gold nanoparticles: Vapor-phase epoxidation of propene with high conversion
    Sinha, AK
    Seelan, S
    Tsubota, S
    Haruta, M
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2004, 43 (12) : 1546 - 1548
  • [40] Three-dimensional mesoporous titanosilicates prepared by modified sol-gel method: Ideal gold catalyst supports for enhanced propene epoxidation
    Sinha, AK
    Seelan, S
    Okumura, M
    Akita, T
    Tsubota, S
    Haruta, M
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (09) : 3956 - 3965