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Catalytic Cleavage of the C-H and C-C Bonds of Alkanes by Surface Organometallic Chemistry: An EXAFS and IR Characterization of a Zr-H Catalyst

Judith Corker, Frédéric Lefebvre, Christine Lécuyer, Véronique Dufaud, Françoise Quignard, Agnès Choplin, John Evans and Jean-Marie Basset
Science
New Series, Vol. 271, No. 5251 (Feb. 16, 1996), pp. 966-969
Stable URL: http://www.jstor.org/stable/2889995
Page Count: 4
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Catalytic Cleavage of the C-H and C-C Bonds of Alkanes by Surface Organometallic Chemistry: An EXAFS and IR Characterization of a Zr-H Catalyst
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Abstract

The catalytic cleavage under hydrogen of the C-H and C-C bonds of alkanes with conventional catalysts requires high temperatures. Room-temperature hydrogenolysis of simple alkanes is possible on a well-defined and well-characterized zirconium hydride supported on silica obtained by surface organometallic chemistry. The surface structure resulting from hydrogenolysis of ($\cong$SiO)Zr(Np)$_3$ (Np, neopentyl) was determined from the extended x-ray absorption fine structure (EXAFS) and $^1$H and $^{29}$Si solid-state nuclear magnetic resonance and infrared (IR) spectra. A mechanism for the formation of ($\cong$SiO)$_3$Zr-H and ($\cong$SiO)$_2$SiH$_2$ and the resulting low-temperature hydrogenolysis of alkanes is proposed. The mechanism may have implications for the catalytic formation of methane, ethane, and lower alkanes in natural gas.

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