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	Structure and hydroformylation performance of supported aqueous-phase Rh catalyst
	Yuan, YZ ; Yuan YZ(袁友珠) ; Zhang, Y ; Zhang Y(张宇) ; Chen, Z ; Chen Z(陈忠) ; Zhang, HB ; Zhang HB(张鸿斌) ; Khirui, T ; Cai QR(蔡启瑞)
	1998
关键词	hydroformylation supported aqueous-phase catalyst MAS NMR P-31 spectroscopy 1-hexene
英文摘要	The catalytic activity of hydroformylation of 1-hexene over SiO2-supported TPPTS-Rh(acac)(CO)(2) (SAPC) was found to be evidently promoted when a proper amount of water-vapor was introduced into the reactant. Characterization results by using: MAS NMR P-31 spectra revealed that there were three types of phosphine species in the as-prepared SAPC: uncoordinated ligand TPPTS (over 70 mol%), surface complex {Rh(CO)(TPPTS)(2)} (chemical shift at delta=32.4, about 15 mol%), and unknown (about 10 mol%). By pre-treatment at 373 K for 2 h under dry-snygas or at 333 K for 2 h under wet-syngas, the amount of phosphine species of the surface complex {Rh(CO)(TPPTS)(2)} was slightly increased to 20-30 mol%, accompanying a few changes in ratios of the other phsophine species. When the SAPC was pre-treated at 373 K for 2 h under wet-syngas, however, the phosphine species at chemical shift of 32.4 was increased by over 40 mol% due to the in-situ formation of the surface complex {Rh(CO)(TPPTS)(2)}. It was found that the peak at delta=32.4 was also a principal one in the MAS NMR P-31 spectra of the working SAPC, which demonstrated that the surface complex of {Rh(CO)(TPPTS)(2)} would be a catalytic active species for olefin hydroformylation. After hydroformylation for 43 h, the deactivation of the catalyst occurred, corresponding to the observations of a broadness in peak ascribed to the surface complex of {Rh(CO)(TPPTS)(2)} in the MAS NMR P-31 spectra, indicating that there existed de-coordination of the surface complex and oxidation of the ligand TPPTS during the reaction. The results suggest that a proper amount of water-vapor was able to accelerate the formation of active Rh-complex on the catalyst surface and thus increase the catalytic activity, whereas, it could be inevitably to cause the de-coordination of the surface complex and the oxidation of phosphine ligand under the reaction condition, hence leading to the deactivation of the catalyst.
语种	中文
出版者	PEKING UNIV PRESS
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/13289]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	Yuan, YZ,Yuan YZ,Zhang, Y,et al. Structure and hydroformylation performance of supported aqueous-phase Rh catalyst[J],1998.
APA	Yuan, YZ.,袁友珠.,Zhang, Y.,张宇.,Chen, Z.,...&蔡启瑞.(1998).Structure and hydroformylation performance of supported aqueous-phase Rh catalyst..
MLA	Yuan, YZ,et al."Structure and hydroformylation performance of supported aqueous-phase Rh catalyst".(1998).

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