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
收藏
页码:2715 / 2729
页数:29
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