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

被引:209
作者
Corker, J
Lefebvre, F
Lecuyer, C
Dufaud, V
Quignard, F
Choplin, A
Evans, J
Basset, JM
机构
[1] ECOLE SUPER CHIM PHYS & ELECTR LYON,CHIM ORGANOMET SURFACE LAB,CNRS,UNITE MIXTE RECH 9986,F-69616 VILLEURBANNE,FRANCE
[2] INST RECH CATALYSE,CNRS,F-69626 VILLEURBANNE,FRANCE
关键词
D O I
10.1126/science.271.5251.966
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 (=SiO)Zr(Np)(3) (Np, neopentyl) was determined from the extended x-ray absorption fine structure (EXAFS) and H-1 and Si-29 solid-state nuclear magnetic resonance and infrared (IR) spectra. A mechanism for the formation of (=SiO)(3)Zr-H and (=SiO)(2)SiH2 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.
引用
收藏
页码:966 / 969
页数:4
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