期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 113, 期 16, 页码 6589-6595出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp810432p
关键词
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资金
- National Natural Science Foundation of China [20673111, 20573106, 20873140]
- Ministry of Science and Technology of China through the National Key Project of Fundamental Research [2009CB623507]
A ligand (triphenyl phosphine, PPh3)-modified heterogeneous PPh3-Rh(CO)/SBA-15 catalyst and supported Wilkinson complex HRh(CO)(PPh3)(3)/SBA-15 catalyst were prepared and examined in the hydroformylation of propene. Heterogeneous PPh3-Rh(CO)/SBA-15 catalyst showed much higher activity and stability in this reaction. Multimuclear H-1, Si-29, P-31, and O-17 MAS NMR and two-dimensional O-17 MQ MAS NMR together with XRD and N-2 adsorption were employed to study the local structures of these two catalysts. Quantitative H-1 and Si-29 MAS NMR and qualitative one- and two-dimensional O-17 MAS and MQ MAS NMR indicate that in the presence of CO the silanols on the surface of SBA-15 can react with rhodium carbonyls to form the Si-O-Rh bonds at the interface between the catalyst and the support. IT MAS NMR spectra demonstrate a similar Wilkinson complex structure is produced on the heterogeneous PPh3-Ph(CO)/SBA-15 catalyst. The formation of Si-O-Rh bonds at the interface may immobilize the Rh complex during the long reaction. These may be correlated to the higher performances of heterogeneous PPh3-Rh(CO)/SBA-15 catalyst in propene hydroformylation.
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