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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