Synthesis, characterization, and catalytic properties of γ-Al 2O3-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations

Jérôme Joubert; Françoise Delbecq; Chloé Thieuleux; Mostafa Taoufik; Frédéric Blanc; Christophe Copéret; Jean Thivolle-Cazat; Jean Marie Basset; Philippe Sautet

doi:10.1021/om070145f

Synthesis, characterization, and catalytic properties of γ-Al ₂O₃-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations

Jérôme Joubert, Françoise Delbecq, Chloé Thieuleux, Mostafa Taoufik, Frédéric Blanc, Christophe Copéret, Jean Thivolle-Cazat, Jean Marie Basset^*, Philippe Sautet

^*Corresponding author for this work

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30 Scopus citations

Abstract

The treatment of the alumina-supported [Zr(CH₂tBu)₄], [(Al_sO)₂Zr(CH₂fBu)⁺(tBuCH ₂)Al_s^-], where Al_s stands for surface aluminum atoms, by H₂ yields a mixture of alumina-supported zirconium hydride species, [(Al_sO)₂Zr(H)(μ-H)Al _VI] and [(Al_sO)₂Zr(H)(μ-R)Al_VI], along with cationic [(Al_sO)₂Zr(H)]⁺ in the vicinity of anionic tetrahedral aluminum hydrides [Al_IV-H ^-] according to mass balance analysis, reactivity studies, IR spectroscopy, and periodic calculations. Initial and final selectivities in the hydrogenolysis of alkanes as well as DFT calculations show that β-alkyl transfer is the key carbon-carbon cleavage step.

Original language	English (US)
Pages (from-to)	3329-3335
Number of pages	7
Journal	Organometallics
Volume	26
Issue number	14
DOIs	https://doi.org/10.1021/om070145f
State	Published - Jul 2 2007
Externally published	Yes

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Organic Chemistry
Inorganic Chemistry

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10.1021/om070145f

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Joubert, J., Delbecq, F., Thieuleux, C., Taoufik, M., Blanc, F., Copéret, C., Thivolle-Cazat, J., Basset, J. M., & Sautet, P. (2007). Synthesis, characterization, and catalytic properties of γ-Al ₂O₃-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations. Organometallics, 26(14), 3329-3335. https://doi.org/10.1021/om070145f

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title = "Synthesis, characterization, and catalytic properties of γ-Al 2O3-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations",

abstract = "The treatment of the alumina-supported [Zr(CH2tBu)4], [(AlsO)2Zr(CH2fBu)+(tBuCH 2)Als-], where Als stands for surface aluminum atoms, by H2 yields a mixture of alumina-supported zirconium hydride species, [(AlsO)2Zr(H)(μ-H)Al VI] and [(AlsO)2Zr(H)(μ-R)AlVI], along with cationic [(AlsO)2Zr(H)]+ in the vicinity of anionic tetrahedral aluminum hydrides [AlIV-H -] according to mass balance analysis, reactivity studies, IR spectroscopy, and periodic calculations. Initial and final selectivities in the hydrogenolysis of alkanes as well as DFT calculations show that β-alkyl transfer is the key carbon-carbon cleavage step.",

author = "J{\'e}r{\^o}me Joubert and Fran{\c c}oise Delbecq and Chlo{\'e} Thieuleux and Mostafa Taoufik and Fr{\'e}d{\'e}ric Blanc and Christophe Cop{\'e}ret and Jean Thivolle-Cazat and Basset, {Jean Marie} and Philippe Sautet",

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Joubert, J, Delbecq, F, Thieuleux, C, Taoufik, M, Blanc, F, Copéret, C, Thivolle-Cazat, J, Basset, JM & Sautet, P 2007, 'Synthesis, characterization, and catalytic properties of γ-Al ₂O₃-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations', Organometallics, vol. 26, no. 14, pp. 3329-3335. https://doi.org/10.1021/om070145f

Synthesis, characterization, and catalytic properties of γ-Al ₂O₃-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations. / Joubert, Jérôme; Delbecq, Françoise; Thieuleux, Chloé et al.
In: Organometallics, Vol. 26, No. 14, 02.07.2007, p. 3329-3335.

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

TY - JOUR

T1 - Synthesis, characterization, and catalytic properties of γ-Al 2O3-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations

AU - Joubert, Jérôme

AU - Delbecq, Françoise

AU - Thieuleux, Chloé

AU - Taoufik, Mostafa

AU - Blanc, Frédéric

AU - Copéret, Christophe

AU - Thivolle-Cazat, Jean

AU - Basset, Jean Marie

AU - Sautet, Philippe

PY - 2007/7/2

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AB - The treatment of the alumina-supported [Zr(CH2tBu)4], [(AlsO)2Zr(CH2fBu)+(tBuCH 2)Als-], where Als stands for surface aluminum atoms, by H2 yields a mixture of alumina-supported zirconium hydride species, [(AlsO)2Zr(H)(μ-H)Al VI] and [(AlsO)2Zr(H)(μ-R)AlVI], along with cationic [(AlsO)2Zr(H)]+ in the vicinity of anionic tetrahedral aluminum hydrides [AlIV-H -] according to mass balance analysis, reactivity studies, IR spectroscopy, and periodic calculations. Initial and final selectivities in the hydrogenolysis of alkanes as well as DFT calculations show that β-alkyl transfer is the key carbon-carbon cleavage step.

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Synthesis, characterization, and catalytic properties of γ-Al ₂O₃-supported zirconium hydrides through a combined use of surface organometallic chemistry and periodic calculations

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