Influence of H2S on ZrO2-based gasification gas clean-up catalysts: MeOH temperature-programmed reaction study

被引：23

作者：

Kauppi, E. Inkeri ^{[1
]}

Ronkkonen, E. Hanne ^{[1
]}

Airaksinen, Sanna M. K. ^{[1
]}

Rasmussen, Soren B. ^{[2
]}

Banares, Miguel A. ^{[2
]}

Krause, A. Outi I. ^{[1
]}

机构：

[1] Aalto Univ, Sch Chem Technol, Dept Biotechnol & Chem Technol, Res Grp Ind Chem, FI-00076 Aalto, Finland

[2] ICP CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2012年 / 111卷

基金：

芬兰科学院;

关键词：

Zirconia catalyst; Effect of H2S; MeOH adsorption; MeOH-DRIFTS; ACTIVE SURFACE SITES; METAL-OXIDES; METHANOL OXIDATION; HYDROGEN-SULFIDE; CARBON-DIOXIDE; ZIRCONIA; ADSORPTION; SULFUR; YTTRIUM; PROBE;

D O I：

10.1016/j.apcatb.2011.11.013

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：

Addition of H2S in the gasification gas stream has been found to improve naphthalene and ammonia conversion over ZrO2 and Y2O3-ZrO2 catalysts, whereas over SiO2-ZrO2 such effect has not been observed. The differences in the properties of the catalysts were studied by spectroscopic (MeOH-DRIFTS) and temperature-programmed methods (H2S-TPD and MeOH-TPSR). Methanol was also used to probe the changes after sulfidation of the catalysts. H2S adsorption sites were found to be different on the ZrO2 and Y2O3-ZrO2 catalysts compared with the ones on the SiO2-ZrO2 catalyst. Sulfur was also found to be more reactive on the ZrO2 and Y2O3-ZrO2 catalysts than on SiO2-ZrO2. It was suggested, that the positive effect of H2S on naphthalene conversion during gasification gas clean-up is connected with the reactions of adsorbed sulfur on their surface. In contrast, on SiO2-ZrO2 the lack of such an effect may be related to limited reactivity of sulfur on the surface. (C) 2011 Elsevier B.V. All rights reserved.

引用

页码：605 / 613

页数：9

共 32 条

[1] Interaction of carbon dioxide with the surface of zirconia polymorphs [J].

Bachiller-Baeza, B ;

Rodriguez-Ramos, I ;

Guerrero-Ruiz, A .

LANGMUIR, 1998, 14 (13) :3556-3564

[2] Methanol: a "smart" chemical probe molecule [J].

Badlani, M ;

Wachs, IE .

CATALYSIS LETTERS, 2001, 75 (3-4) :137-149

[3] INTERMEDIATE SPECIES ON ZIRCONIA SUPPORTED METHANOL AEROGEL CATALYSTS .5. ADSORPTION OF METHANOL [J].

BIANCHI, D ;

CHAFIK, T ;

KHALFALLAH, M ;

TEICHNER, SJ .

APPLIED CATALYSIS A-GENERAL, 1995, 123 (01) :89-110

[4] An X-ray photoelectron spectroscopy study of the acidity of SiO2-ZrO2 mixed oxides [J].

Bosman, HJM ;

Pijpers, AP ;

Jaspers, AWMA .

JOURNAL OF CATALYSIS, 1996, 161 (02) :551-559

[5] Quantitative determination of the number of active surface sites and the turnover frequencies for methanol oxidation over metal oxide catalysts - I. Fundamentals of the methanol chemisorption technique and application to monolayer supported molybdenum oxide catalysts [J].

Briand, LE ;

Farneth, WE ;

Wachs, IE .

CATALYSIS TODAY, 2000, 62 (2-3) :219-229

[6] Infrared studies of the reactive adsorption of organic molecules over metal oxides and of the mechanisms of their heterogeneously-catalyzed oxidation [J].

Busca, G .

CATALYSIS TODAY, 1996, 27 (3-4) :457-496

[7] Hydrogen from alcohols: IR and flow reactor studies [J].

Busca, Guido ;

Montanari, Tania ;

Resini, Carlo ;

Ramis, Gianguido ;

Costantino, Umberto .

CATALYSIS TODAY, 2009, 143 (1-2) :2-8

[8] A surface study of monoclinic zirconia (m-ZrO2) [J].

Cerrato, G ;

Bordiga, S ;

Barbera, S ;

Morterra, C .

SURFACE SCIENCE, 1997, 377 (1-3) :50-55

[9]

Cortez GG, 2003, CATAL TODAY, V78, P219

[10] CLAUS CATALYSIS .2. AN FTIR STUDY OF THE ADSORPTION OF H2S ON THE ALUMINA CATALYST [J].

DATTA, A ;

CAVELL, RG .

JOURNAL OF PHYSICAL CHEMISTRY, 1985, 89 (03) :450-454

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