Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst

Nicolas Merle; Frédéric Le Quéméner; Yassine Bouhoute; Kai C. Szeto; Aimery De Mallmann; Samir Barman; Manoja Samantaray; Laurent Delevoye; Régis M. Gauvin; Mostafa Taoufik; Jean-Marie Basset

doi:10.1021/jacs.6b11220

Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst

Nicolas Merle, Frédéric Le Quéméner, Yassine Bouhoute, Kai C. Szeto, Aimery De Mallmann, Samir Barman, Manoja Samantaray, Laurent Delevoye, Régis M. Gauvin, Mostafa Taoufik, Jean-Marie Basset

Research output: Contribution to journal › Article › peer-review

39 Scopus citations

Abstract

The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH Bu) was selectively prepared by grafting of MoO(CH Bu)Cl onto partially dehydroxylated silica (silica) using the surface organometallic chemistry approach. This surface species was fully characterized by elemental analysis and DRIFT, solid-state NMR, and EXAFS spectroscopy. This new material is related to the active species of industrial supported MoO/SiO olefin metathesis catalysts. It displays very high activity in propene self-metathesis at mild (turnover number = 90 000 after 25 h). Remarkably, its catalytic performance outpaces those of the parent imido derivative and its tungsten oxo analogue.

Original language	English (US)
Pages (from-to)	2144-2147
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	139
Issue number	6
DOIs	https://doi.org/10.1021/jacs.6b11220
State	Published - Feb 6 2017

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): 2174 CGR3
Acknowledgements: We thank the Competitive Research Grant Program, supported by the KAUST Research Fund (Project 2174 CGR3), and the Agence Nationale de la Recherche (ANR-12-BS07-0021-01, OXOCAT) for their financial support and Olivier Mathon for his help during the recording of the XAS spectra on beamline BM23 at ESRF (experiment code IN-986).

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Merle, N., Le Quéméner, F., Bouhoute, Y., Szeto, K. C., De Mallmann, A., Barman, S., Samantaray, M., Delevoye, L., Gauvin, R. M., Taoufik, M., & Basset, J-M. (2017). Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst. Journal of the American Chemical Society, 139(6), 2144-2147. https://doi.org/10.1021/jacs.6b11220

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title = "Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst",

abstract = "The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH Bu) was selectively prepared by grafting of MoO(CH Bu)Cl onto partially dehydroxylated silica (silica) using the surface organometallic chemistry approach. This surface species was fully characterized by elemental analysis and DRIFT, solid-state NMR, and EXAFS spectroscopy. This new material is related to the active species of industrial supported MoO/SiO olefin metathesis catalysts. It displays very high activity in propene self-metathesis at mild (turnover number = 90 000 after 25 h). Remarkably, its catalytic performance outpaces those of the parent imido derivative and its tungsten oxo analogue.",

author = "Nicolas Merle and {Le Qu{\'e}m{\'e}ner}, Fr{\'e}d{\'e}ric and Yassine Bouhoute and Szeto, {Kai C.} and {De Mallmann}, Aimery and Samir Barman and Manoja Samantaray and Laurent Delevoye and Gauvin, {R{\'e}gis M.} and Mostafa Taoufik and Jean-Marie Basset",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): 2174 CGR3 Acknowledgements: We thank the Competitive Research Grant Program, supported by the KAUST Research Fund (Project 2174 CGR3), and the Agence Nationale de la Recherche (ANR-12-BS07-0021-01, OXOCAT) for their financial support and Olivier Mathon for his help during the recording of the XAS spectra on beamline BM23 at ESRF (experiment code IN-986).",

year = "2017",

month = feb,

day = "6",

doi = "10.1021/jacs.6b11220",

language = "English (US)",

volume = "139",

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journal = "Journal of the American Chemical Society",

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Merle, N, Le Quéméner, F, Bouhoute, Y, Szeto, KC, De Mallmann, A, Barman, S, Samantaray, M, Delevoye, L, Gauvin, RM, Taoufik, M & Basset, J-M 2017, 'Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst', Journal of the American Chemical Society, vol. 139, no. 6, pp. 2144-2147. https://doi.org/10.1021/jacs.6b11220

Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst. / Merle, Nicolas; Le Quéméner, Frédéric; Bouhoute, Yassine et al.

In: Journal of the American Chemical Society, Vol. 139, No. 6, 06.02.2017, p. 2144-2147.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst

AU - Merle, Nicolas

AU - Le Quéméner, Frédéric

AU - Bouhoute, Yassine

AU - Szeto, Kai C.

AU - De Mallmann, Aimery

AU - Barman, Samir

AU - Samantaray, Manoja

AU - Delevoye, Laurent

AU - Gauvin, Régis M.

AU - Taoufik, Mostafa

AU - Basset, Jean-Marie

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): 2174 CGR3 Acknowledgements: We thank the Competitive Research Grant Program, supported by the KAUST Research Fund (Project 2174 CGR3), and the Agence Nationale de la Recherche (ANR-12-BS07-0021-01, OXOCAT) for their financial support and Olivier Mathon for his help during the recording of the XAS spectra on beamline BM23 at ESRF (experiment code IN-986).

PY - 2017/2/6

Y1 - 2017/2/6

N2 - The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH Bu) was selectively prepared by grafting of MoO(CH Bu)Cl onto partially dehydroxylated silica (silica) using the surface organometallic chemistry approach. This surface species was fully characterized by elemental analysis and DRIFT, solid-state NMR, and EXAFS spectroscopy. This new material is related to the active species of industrial supported MoO/SiO olefin metathesis catalysts. It displays very high activity in propene self-metathesis at mild (turnover number = 90 000 after 25 h). Remarkably, its catalytic performance outpaces those of the parent imido derivative and its tungsten oxo analogue.

AB - The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH Bu) was selectively prepared by grafting of MoO(CH Bu)Cl onto partially dehydroxylated silica (silica) using the surface organometallic chemistry approach. This surface species was fully characterized by elemental analysis and DRIFT, solid-state NMR, and EXAFS spectroscopy. This new material is related to the active species of industrial supported MoO/SiO olefin metathesis catalysts. It displays very high activity in propene self-metathesis at mild (turnover number = 90 000 after 25 h). Remarkably, its catalytic performance outpaces those of the parent imido derivative and its tungsten oxo analogue.

UR - http://hdl.handle.net/10754/623242

UR - http://pubs.acs.org/doi/full/10.1021/jacs.6b11220

UR - http://www.scopus.com/inward/record.url?scp=85013030276&partnerID=8YFLogxK

U2 - 10.1021/jacs.6b11220

DO - 10.1021/jacs.6b11220

M3 - Article

C2 - 28165238

SN - 0002-7863

VL - 139

SP - 2144

EP - 2147

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 6

ER -

Well-Defined Molybdenum Oxo Alkyl Complex Supported on Silica by Surface Organometallic Chemistry: A Highly Active Olefin Metathesis Precatalyst

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