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
相关论文
共 50 条
  • [1] Silica-Supported Tungsten Neosilyl Oxo Precatalysts: Impact of the Podality on Activity and Stability in Olefin Metathesis
    Grekov, D.
    Bouhoute, Y.
    Szeto, K. C.
    Merle, N.
    De Mallmann, A.
    Lefebvre, F.
    Lucas, C.
    Del Rosa, I.
    Maron, L.
    Gauvin, R. M.
    Delevoye, L.
    Taoufik, M.
    ORGANOMETALLICS, 2016, 35 (13) : 2188 - 2196
  • [2] Quantitatively Analyzing Metathesis Catalyst Activity and Structural Features in Silica-Supported Tungsten Imido-Alkylidene Complexes
    Mougel, Victor
    Santiago, Celine B.
    Zhizhko, Pavel A.
    Bess, Elizabeth N.
    Varga, Jeno
    Frater, Georg
    Sigman, Matthew S.
    Coperet, Christophe
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (20) : 6699 - 6704
  • [3] Well-Defined Silica-Supported Tungsten(IV)-Oxo Complex: Olefin Metathesis Activity, Initiation, and Role of Bronsted Acid Sites
    Chan, Ka Wing
    Mance, Deni
    Safonova, Olga V.
    Coperet, Christophe
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (45) : 18286 - 18292
  • [4] Olefin-Surface Interactions: A Key Activity Parameter in Silica-Supported Olefin Metathesis Catalysts
    Berkson, Zachariah J.
    Bernhardt, Moritz
    Schlapansky, Simon L.
    Benedikter, Mathis J.
    Buchmeiser, Michael R.
    Price, Gregory A.
    Sunley, Glenn J.
    Coperet, Christophe
    JACS AU, 2022, 2 (03): : 777 - 786
  • [5] Silica-supported Z-selective Ru olefin metathesis catalysts
    Renom-Carrasco, Marc
    Mania, Philipp
    Sayah, Reine
    Veyre, Laurent
    Occhipinti, Giovanni
    Jensen, Vidar R.
    Thieuleux, Chloe
    MOLECULAR CATALYSIS, 2020, 483 (483)
  • [6] Insights into Dopant-Mediated Tuning of Silica-Supported Mo Metal Centers for Enhanced Olefin Metathesis
    Uchagawkar, Anoop
    Ramanathan, Anand
    Zhu, Hongda
    Chen, Linxiao
    Hu, Yongfeng
    Douglas, Justin
    Mais, Marco
    Kobayashi, Takeshi
    Subramaniam, Bala
    ACS CATALYSIS, 2024, 14 (11): : 8317 - 8329
  • [7] Modification of silica-supported tungsten neosilyl oxo precatalysts: impact of substituted phenol on activity and stability in olefin metathesis
    Bouhoute, Y.
    Del Rosal, I.
    Szeto, K. C.
    Merle, N.
    Grekov, D.
    De Mallmann, A.
    Le Roux, E.
    Delevoye, L.
    Gauvin, R. M.
    Maron, L.
    Taoufik, M.
    CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (24) : 8532 - 8539
  • [8] Imine Metathesis Catalyzed by a Silica-Supported Hafnium Imido Complex
    Aljuhani, Maha A.
    Barman, Samir
    Abou-Hamad, Edy
    Gurinov, Andrei
    Ould-Chikh, Samy
    Guan, Erjia
    Jedidi, Abdesslem
    Cavallo, Luigi
    Gates, Bruce C.
    Pelletier, Jeremie D. A.
    Basset, Jean-Marie
    ACS CATALYSIS, 2018, 8 (10): : 9440 - 9446
  • [9] On the Track to Silica-Supported Tungsten Oxo Metathesis Catalysts: Input from 17O Solid-State NMR
    Merle, Nicolas
    Girard, Guillaume
    Popoff, Nicolas
    De Mallmann, Aimery
    Bouhoute, Yassine
    Trebosc, Julien
    Berrier, Elise
    Paul, Jean-Francois
    Nicholas, Christopher P.
    Del Rosal, Iker
    Maron, Laurent
    Gauvin, Regis M.
    Delevoye, Laurent
    Taoufik, Mostafa
    INORGANIC CHEMISTRY, 2013, 52 (17) : 10119 - 10130
  • [10] Silica-Supported Cationic Tungsten Imido Alkylidene Stabilized by an N-Heterocyclic Carbene Ligand Boosts Activity and Selectivity in the Metathesis of α-Olefins
    De Jesus Silva, Jordan
    Mance, Deni
    Pucino, Margherita
    Benedikter, Mathis J.
    Elser, Iris
    Buchmeiser, Michael R.
    Coperet, Christophe
    HELVETICA CHIMICA ACTA, 2020, 103 (11)
12345