What drives the selectivity for CO methanation in the methanation of CO2-rich reformate gases on supported Ru catalysts?

被引：52

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：

APPLIED CATALYSIS A-GENERAL | 2011年 / 391卷 / 1-2期

关键词：

Selective methanation; CO methanation; Mechanism; CO adsorption; Ru catalyst; CARBON-MONOXIDE; HETEROGENEOUS CATALYSIS; INFRARED-SPECTRA; HYDROGEN; ADSORPTION; RU/TIO2; FTIR; IR; HYDROCARBONS; COADSORPTION;

D O I：

10.1016/j.apcata.2010.07.025

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 their selectivity for CO methanation and the underlying physical reasons, we have investigated the selective methanation of CO over two supported Ru catalysts, a Ru/zeolite catalyst and a Ru/Al2O3 catalyst, in CO2-rich reformate gases by combined kinetic and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements. Based on the correlation between COad band intensity/COad coverage and the selectivity for CO methanation over a wide range of CO contents, down to 100 ppm, two different mechanisms are identified for the two catalysts. On Ru/Al2O3, the selectivity results from blocking of active surface sites by adsorbed CO, while for the Ru/zeolite catalyst we relate this to an inherently low activity of the very small Ru nanoparticles for CO2 dissociation and subsequent methanation. The underlying reasons and consequences for practical applications are discussed. (C) 2010 Elsevier B.V. All rights reserved.

引用

页码：325 / 333

页数：9

共 53 条

[1] Structure sensitivity of the methanation reaction:: H2-induced CO dissociation on nickel surfaces [J].

Andersson, M. P. ;

Abild-Pedersen, F. ;

Remediakis, I. N. ;

Bligaard, T. ;

Jones, G. ;

Engbwk, J. ;

Lytken, O. ;

Horch, S. ;

Nielsen, J. H. ;

Sehested, J. ;

Rostrup-Nielsen, J. R. ;

Norskov, J. K. ;

Chorkendorff, I. .

JOURNAL OF CATALYSIS, 2008, 255 (01) :6-19

[2] Toward computational screening in heterogeneous catalysis: Pareto-optimal methanation catalysts [J].

Andersson, MP ;

Bligaard, T ;

Kustov, A ;

Larsen, KE ;

Greeley, J ;

Johannessen, T ;

Christensen, CH ;

Norskov, JK .

JOURNAL OF CATALYSIS, 2006, 239 (02) :501-506

[3] The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis [J].

Bligaard, T ;

Norskov, JK ;

Dahl, S ;

Matthiesen, J ;

Christensen, CH ;

Sehested, J .

JOURNAL OF CATALYSIS, 2004, 224 (01) :206-217

[4] Acid and basic catalysis [J].

Bronsted, JN .

CHEMICAL REVIEWS, 1928, 5 (03) :231-338

[5] INFRARED STUDY OF ADSORPTION OF CARBON-MONOXIDE ON REDUCED AND OXIDIZED FORMS OF SILICA SUPPORTED RUTHENIUM [J].

BROWN, MF ;

GONZALEZ, RD .

JOURNAL OF PHYSICAL CHEMISTRY, 1976, 80 (15) :1731-1735

[6] Preferential methanation of CO in a syngas involving CO2 at lower temperature range [J].

Choudhury, Muhamad B. I. ;

Ahmed, Shakeel ;

Shalabi, Mazen A. ;

Inui, Tomoyuki .

APPLIED CATALYSIS A-GENERAL, 2006, 314 (01) :47-53

[7] SOME GENERAL-ASPECTS OF HYDROGEN CHEMISORPTION ON METAL-SURFACES [J].

CHRISTMANN, K .

PROGRESS IN SURFACE SCIENCE, 1995, 48 (1-4) :15-26

[8] Selective CO methanation catalysts for fuel processing applications [J].

Dagle, Robert A. ;

Wang, Yong ;

Xia, Guan-Guang ;

Strohm, James J. ;

Holladay, Jamelyn ;

Palo, Daniel R. .

APPLIED CATALYSIS A-GENERAL, 2007, 326 (02) :213-218

[9]

DALLABETTA RA, 1977, J CATAL, V48, P111

[10] IR STUDY OF NO AND CO ADSORPTION ON A SILICA-SUPPORTED RU CATALYST [J].

DAVYDOV, AA ;

BELL, AT .

JOURNAL OF CATALYSIS, 1977, 49 (03) :332-344

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