A Silica-Supported Monoalkylated Tungsten Dioxo Complex Catalyst for Olefin Metathesis

被引：44

作者：

Maity, Niladri ^{[1
]}

Barman, Samir ^{[1
]}

Minenkov, Yury ^{[1
]}

Ould-Chikh, Samy ^{[1
]}

Abou-Hamad, Edy ^{[1
]}

Ma, Tao ^{[2
]}

Qureshi, Ziyauddin S. ^{[1
,3
]}

Cavallo, Luigi ^{[1
]}

D'Elia, Valerio ^{[1
,4
]}

Gates, Bruce C. ^{[2
]}

Basset, Jean-Marie ^{[1
]}

机构：

[1] King Abdullah Univ Sci & Technol, KCC, Thuwal 239556900, Saudi Arabia

[2] Univ Calif Davis, Dept Chem Engn, Davis, CA 95616 USA

[3] King Fahd Univ Petr & Minerals, Ctr Res Excellence Petr Refining & Petrochem, Dhahran 31261, Saudi Arabia

[4] Vidyasirimedhi Inst Sci & Technol VISTEC, Sch Mol Sci & Engn, Dept Mat Sci & Engn, Wangchan 21210, Rayong, Thailand

来源：

ACS CATALYSIS | 2018年 / 8卷 / 04期

关键词：

olefin metathesis; tungsten dioxo complex; mechanistic study; metallacyclobutane intermediate; tungsten alkylidene; SINGLE-SITE; OXO ALKYLIDENE; ACTIVE-SITES; METALLACYCLOBUTANE COMPLEXES; PERTURBATION-THEORY; PROPENE METATHESIS; HIGHLY EFFICIENT; OXIDE CATALYSTS; SURFACE; SPECTROSCOPY;

D O I：

10.1021/acscatal.7b04304

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：

A well-defined silica-supported monoalkylated tungsten dioxo complex [( Si-O-)W(=O)(2)(CH2-Bu-t)] was prepared by treatment of highly dehydroxylated silica (SiO2-700: silica treated at 700 degrees C under high vacuum) with an ionic precursor complex [NEt4][W(=O)(3)(CH2-Bu-t)]. The identity of the resulting neutral monoalkylated tungsten dioxo surface complex was established by means of elemental microanalysis and spectroscopic studies (IR, solid-state NMR, Raman, and X-ray absorption spectroscopies). The supported tungsten dioxo tungsten complex was found to act as a precatalyst for the self-metathesis of 1-octene in a batch reactor. The mechanistic implications of this reaction are discussed with the support of DFT calculations highlighting the potential occurrence of thus-far unexplored mechanistic pathways.

引用

页码：2715 / 2729

页数：29

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