Well-Defined Supported Mononuclear Tungsten Oxo Species as Olefin Metathesis Pre-Catalysts

被引:39
作者
Bouhoute, Yassine [1 ]
Garron, Anthony [1 ]
Grekov, Denys [2 ]
Merle, Nicolas [1 ]
Szeto, Kai C. [1 ]
De Mallmann, Aimery [1 ]
Del Rosal, Iker [3 ]
Maron, Laurent [3 ]
Girard, Guillaume [2 ]
Gauvin, Regis M. [2 ]
Delevoye, Laurent [2 ]
Taoufik, Mostafa [1 ]
机构
[1] UCBL, ESCPE Lyon, Lab Chim Catalyse Polymeres & Proc, CNRS,UMR 5265, F-69616 Villeurbanne, France
[2] Univ Lille, CNRS UMR 8181, Unite Catalyse & Chim Solide, F-59655 Villeneuve Dascq, France
[3] Univ Toulouse, INSA, Lab Physicochim Nanoobjets, CNRS,UMR 5215,UPS, F-31077 Toulouse, France
关键词
metathesis; surface chemistry; tungsten; tin; alkylation; GENERALIZED GRADIENT APPROXIMATION; GRAFTED LANTHANIDE COMPLEXES; RING-OPENING POLYMERIZATION; RAY CRYSTAL-STRUCTURE; BASIS-SETS; EPSILON-CAPROLACTONE; PERTURBATION-THEORY; ALKENE METATHESIS; REACTIVITY; EXCHANGE;
D O I
10.1021/cs501294j
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
[WOCl4] was grafted on silica dehydroxylated at 200 degrees C, and the structure of the surface species was elucidated by a combination of spectroscopic and theoretical methods, demonstrating the formation of [( SiO)(2)WOCl2] (1a) as the major species accompanied by minor monopodal species [( SiO)WOCl3] (1b). Most noteworthy, EXAFS and O-17 NMR combined to DFT calculations helped elucidate the structure of the surface species. Alkylation was performed using SnMe4, affording methyl species that were also precisely characterized. The alkylated species achieved excellent performances in isobutene metathesis to 2,3-dimethylbutene.
引用
收藏
页码:4232 / 4241
页数:10
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