DICP OpenIR
Oxidative steam reforming of ethanol over Ir/CeO2 catalysts: A structure sensitivity analysis
Cai, Weijie2; Wang, Fagen1; Daniel, Cecile2; van Veen, Andre C.2,3; Schuurman, Yves2; Descorme, Claude2; Provendier, Helene2; Shen, Wenjie1; Mirodatos, Claude2
KeywordOxidative Steam Reforming Ethanol Iridium Ceria Hydrogen Production Structure Sensitivity
Source PublicationJOURNAL OF CATALYSIS
2012-02-01
DOI10.1016/j.jcat.2011.10.021
Volume286Pages:137-152
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
WOS SubjectChemistry, Physical ; Engineering, Chemical
WOS Research AreaChemistry ; Engineering
WOS KeywordSUPPORTED PALLADIUM CATALYSTS ; O-18/O-16 ISOTOPIC EXCHANGE ; BIOMASS-DERIVED ETHANOL ; FUEL-CELL APPLICATIONS ; METAL BASED CATALYSTS ; NI-BASED CATALYSTS ; HYDROGEN-PRODUCTION ; BIO-ETHANOL ; REACTION-MECHANISM ; SURFACE MOBILITY
AbstractA series of Ir/CeO2 catalysts of different oxide and metallic phase dispersions was investigated by XRD, TPR, HRTEM, CO2 TPD/calorimetry, in situ DRIFT spectroscopy, and oxygen isotopic exchange techniques in order to elucidate the specific influence of catalyst morphology and structure on the oxidative steam reforming (OSR) of ethanol. Structure/texture sensitivity is demonstrated on the basis of the OSR mechanism, which involves, in order: (i) ethanol adsorption on the ceria surface, (ii) partial oxidation to acetate and surface migration of the C2 intermediates along the ceria support toward the Ir particles. (iii) cracking and further oxidation into Ir carbonyls and ceria carbonates, and (iv) hydrogen and carbon monoxide desorption from the Ir particles. Structure sensitivity is established by considering two types of sites: the ceria surface sites, which are essentially pairs of oxygen vacancies and basic OH groups, as well as interfacial sites between Ir and ceria phases, involving pairs of Ir coordinately unsaturated sites (CUSs) and the aforementioned Peripheral ceria sites. This structure sensitivity is revealed by TOF calculations based on these two types of sites, which correspond to the two main rate controlling steps of the ethanol OSR mechanism, namely steps (ii) and (iii). The materials considered display activity, selectivity, and resistance to aging (manifested by coke deposition and sintering) that are closely related to their initial structure and texture. Two domains in terms of iridium and ceria particle size are identified, leading either to stable and selective catalysts or to unstable and unselective catalysts. Such an original and quantified structure sensitivity analysis should prove useful for further process development. (C) 2011 Published by Elsevier Inc.
Language英语
WOS IDWOS:000300141300015
Citation statistics
Cited Times:72[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/142984
Collection中国科学院大连化学物理研究所
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Univ Lyon 1, CNRS, Inst Rech Catalyse & Environm Lyon IRCELYON, UMR 5256, F-69626 Villeurbanne, France
3.Ruhr Univ Bochum, Lab Ind Chem, D-44780 Bochum, Germany
Recommended Citation
GB/T 7714
Cai, Weijie,Wang, Fagen,Daniel, Cecile,et al. Oxidative steam reforming of ethanol over Ir/CeO2 catalysts: A structure sensitivity analysis[J]. JOURNAL OF CATALYSIS,2012,286:137-152.
APA Cai, Weijie.,Wang, Fagen.,Daniel, Cecile.,van Veen, Andre C..,Schuurman, Yves.,...&Mirodatos, Claude.(2012).Oxidative steam reforming of ethanol over Ir/CeO2 catalysts: A structure sensitivity analysis.JOURNAL OF CATALYSIS,286,137-152.
MLA Cai, Weijie,et al."Oxidative steam reforming of ethanol over Ir/CeO2 catalysts: A structure sensitivity analysis".JOURNAL OF CATALYSIS 286(2012):137-152.
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