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 K. 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 K. Samantaray, Laurent Delevoye, Régis M. Gauvin, Mostafa Taoufik, Jean Marie Basset

^*Corresponding author for this work

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

55 Scopus citations

Abstract

The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH₂^tBu)₃ was selectively prepared by grafting of MoO(CH₂^tBu)₃Cl onto partially dehydroxylated silica (silica₇₀₀) 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 MoO₃/SiO₂ 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
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 - 15 Feb 2017
Externally published	Yes

Bibliographical note

Funding Information:
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).

Publisher Copyright:
© 2016 American Chemical Society.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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Merle, N., Le Quéméner, F., Bouhoute, Y., Szeto, K. C., De Mallmann, A., Barman, S., Samantaray, M. K., 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(CH2tBu)3 was selectively prepared by grafting of MoO(CH2tBu)3Cl onto partially dehydroxylated silica (silica700) 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 MoO3/SiO2 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 Samantaray, \{Manoja K.\} and Laurent Delevoye and Gauvin, \{R{\'e}gis M.\} and Mostafa Taoufik and Basset, \{Jean Marie\}",

note = "Funding Information: 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). Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2017",

month = feb,

day = "15",

doi = "10.1021/jacs.6b11220",

language = "English",

volume = "139",

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Merle, N, Le Quéméner, F, Bouhoute, Y, Szeto, KC, De Mallmann, A, Barman, S, Samantaray, MK, Delevoye, L, Gauvin, RM, Taoufik, M & Basset, JM 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, 15.02.2017, 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

T2 - 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 K.

AU - Delevoye, Laurent

AU - Gauvin, Régis M.

AU - Taoufik, Mostafa

AU - Basset, Jean Marie

N1 - Funding Information: 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). Publisher Copyright: © 2016 American Chemical Society.

PY - 2017/2/15

Y1 - 2017/2/15

N2 - The well-defined silica-supported molybdenum oxo alkyl species (SiO−)MoO(CH2tBu)3 was selectively prepared by grafting of MoO(CH2tBu)3Cl onto partially dehydroxylated silica (silica700) 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 MoO3/SiO2 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(CH2tBu)3 was selectively prepared by grafting of MoO(CH2tBu)3Cl onto partially dehydroxylated silica (silica700) 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 MoO3/SiO2 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 - https://www.scopus.com/pages/publications/85013030276

U2 - 10.1021/jacs.6b11220

DO - 10.1021/jacs.6b11220

M3 - Article

C2 - 28165238

AN - SCOPUS:85013030276

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

Abstract

Bibliographical note

ASJC Scopus subject areas

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