Controlling the hydrogenolysis of silica-supported tungsten pentamethyl leads to a class of highly electron deficient partially alkylated metal hydrides
Abstract
The well-defined single-site silica-supported tungsten complex [(Si–O–)W(Me)5], 1, is an excellent precatalyst for alkane metathesis. The unique structure of 1 allows the synthesis of unprecedented tungsten hydrido methyl surface complexes via a controlled hydrogenolysis. Specifically, in the presence of molecular hydrogen, 1 is quickly transformed at -78 °C into a partially alkylated tungsten hydride, 4, as characterized by 1H solid-state NMR and IR spectroscopies. Species 4, upon warming to 150 °C, displays the highest catalytic activity for propane metathesis yet reported. DFT calculations using model systems support the formation of [(Si–O–)WH3(Me)2], as the predominant species at -78 °C following several elementary steps of hydrogen addition (by σ-bond metathesis or α-hydrogen transfer). Rearrangement of 4 occuring between -78 °C and room temperature leads to the formation of an unique methylidene tungsten hydride [(Si–O–)WH3(CH2)], as determined by solid-state 1H and 13C NMR spectroscopies and supported by DFT. Thus for the first time, a coordination sphere that incorporates both carbene and hydride functionalities has been observed.
- Authors:
-
- King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia). KAUST Catalysis Center (KCC)
- King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia). KAUST Catalysis Center (KCC); Vidyasirimedhi Inst. of Science and Technology, Rayong (Thailand). Dept. of Materials Science and Engineering
- Univ. of California, Davis, CA (United States). Dept. of Chemical Engineering and Materials Science
- Durham Univ. (United Kingdom). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Univ. of California, Davis, CA (United States); King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Sciences and Engineering Research Council of Canada (NSERC); King Abdullah Univ. of Science and Technology (Saudi Arabia)
- OSTI Identifier:
- 1439325
- Grant/Contract Number:
- FG02-04ER15513
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Maity, Niladri, Barman, Samir, Callens, Emmanuel, Samantaray, Manoja K., Abou-Hamad, Edy, Minenkov, Yury, D'Elia, Valerio, Hoffman, Adam S., Widdifield, Cory M., Cavallo, Luigi, Gates, Bruce C., and Basset, Jean-Marie. Controlling the hydrogenolysis of silica-supported tungsten pentamethyl leads to a class of highly electron deficient partially alkylated metal hydrides. United States: N. p., 2015.
Web. doi:10.1039/c5sc03490f.
Maity, Niladri, Barman, Samir, Callens, Emmanuel, Samantaray, Manoja K., Abou-Hamad, Edy, Minenkov, Yury, D'Elia, Valerio, Hoffman, Adam S., Widdifield, Cory M., Cavallo, Luigi, Gates, Bruce C., & Basset, Jean-Marie. Controlling the hydrogenolysis of silica-supported tungsten pentamethyl leads to a class of highly electron deficient partially alkylated metal hydrides. United States. https://doi.org/10.1039/c5sc03490f
Maity, Niladri, Barman, Samir, Callens, Emmanuel, Samantaray, Manoja K., Abou-Hamad, Edy, Minenkov, Yury, D'Elia, Valerio, Hoffman, Adam S., Widdifield, Cory M., Cavallo, Luigi, Gates, Bruce C., and Basset, Jean-Marie. Mon .
"Controlling the hydrogenolysis of silica-supported tungsten pentamethyl leads to a class of highly electron deficient partially alkylated metal hydrides". United States. https://doi.org/10.1039/c5sc03490f. https://www.osti.gov/servlets/purl/1439325.
@article{osti_1439325,
title = {Controlling the hydrogenolysis of silica-supported tungsten pentamethyl leads to a class of highly electron deficient partially alkylated metal hydrides},
author = {Maity, Niladri and Barman, Samir and Callens, Emmanuel and Samantaray, Manoja K. and Abou-Hamad, Edy and Minenkov, Yury and D'Elia, Valerio and Hoffman, Adam S. and Widdifield, Cory M. and Cavallo, Luigi and Gates, Bruce C. and Basset, Jean-Marie},
abstractNote = {The well-defined single-site silica-supported tungsten complex [(Si–O–)W(Me)5], 1, is an excellent precatalyst for alkane metathesis. The unique structure of 1 allows the synthesis of unprecedented tungsten hydrido methyl surface complexes via a controlled hydrogenolysis. Specifically, in the presence of molecular hydrogen, 1 is quickly transformed at -78 °C into a partially alkylated tungsten hydride, 4, as characterized by 1H solid-state NMR and IR spectroscopies. Species 4, upon warming to 150 °C, displays the highest catalytic activity for propane metathesis yet reported. DFT calculations using model systems support the formation of [(Si–O–)WH3(Me)2], as the predominant species at -78 °C following several elementary steps of hydrogen addition (by σ-bond metathesis or α-hydrogen transfer). Rearrangement of 4 occuring between -78 °C and room temperature leads to the formation of an unique methylidene tungsten hydride [(Si–O–)WH3(CH2)], as determined by solid-state 1H and 13C NMR spectroscopies and supported by DFT. Thus for the first time, a coordination sphere that incorporates both carbene and hydride functionalities has been observed.},
doi = {10.1039/c5sc03490f},
journal = {Chemical Science},
number = 2,
volume = 7,
place = {United States},
year = {Mon Nov 30 00:00:00 EST 2015},
month = {Mon Nov 30 00:00:00 EST 2015}
}
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