Reaction Intermediates and Side Products in the Methanation of CO and CO2 over Supported Ru Catalysts in H2-Rich Reformate Gases

被引：233

作者：

Eckle, Stephan ^{[1
]}

Anfang, Hans-Georg ^{[2
]}

Behm, R. Juergen ^{[1
]}

机构：

[1] Univ Ulm, Inst Catalysis & Surface Chem, D-89069 Ulm, Germany

[2] Sud Chem AG, R&D Energy & Environm, D-83502 Bruckmuhl, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2011年 / 115卷 / 04期

关键词：

SINGLE-CRYSTAL NICKEL; CARBON-MONOXIDE; INFRARED-SPECTRA; HYDROGENATION; FTIR; HYDROCARBONS; COADSORPTION; ADSORPTION; MECHANISM; SURFACE;

D O I：

10.1021/jp108106t

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Aiming at a mechanistic understanding of the CO and CO2 methanation reaction over supported Ru catalysts and the underlying physical reasons, we have investigated the methanation of CO and CO2 over a Ru/zeolite and a Ru/Al2O3 catalyst, in idealized and CO2-rich reformate gases by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements, employing quantitative steady-state isotope transient kinetik analysis (SSITKA) techniques. On the basis of the correlation between COad band intensity/COad kcoverage, CH4,ad/HCOad/formate band intensity, and the CH4 formation rate under steady-state conditions, HCOad is unambiguously identified as reaction intermediate species in the dominant reaction pathway for CO methanation on the Ru/Al2O3 catalyst. On the Ru/zeolite such species could not be detected. CO2 methanation proceeds via dissociation to COad, which is subsequently methanated. Formation and decomposition of surface formates plays only a minor role in the latter reaction, they rather act as spectator species.

引用

页码：1361 / 1367

页数：7

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