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Heats of adsorption of linear CO species adsorbed on reduced Fe/Al2O3 catalysts using the AEIR method in diffuse reflectance mode

Paper ID Volume ID Publish Year Pages File Format Full-Text
41054 45876 2011 11 PDF Available
Title
Heats of adsorption of linear CO species adsorbed on reduced Fe/Al2O3 catalysts using the AEIR method in diffuse reflectance mode
Abstract

IR spectra in diffuse reflectance mode are quantitatively exploited to determine the heats of adsorption of two linearly adsorbed CO species formed on Fe2+ and Fe° sites (denoted LFe2+LFe2+ and LFe° CO species) of reduced x% Fe/Al2O3 (wt%, x = 1 and 5) catalysts according to the AEIR procedure developed previously using the IR transmission mode. The IR transmission properties of iron containing catalysts are limited particularly for high iron loadings favoring the use of the diffuse reflectance mode. The heats of adsorption of the LFe2+LFe2+ CO species linearly vary with the coverage of the sites from ELFe2+(1)=45 kJ/molELFe2+(1)=45 kJ/mol to ELFe2+(0)=66 kJ/molELFe2+(0)=66 kJ/mol at coverage 1 and 0, respectively. These values are modified by the presence of neither Fe° sites nor carbonaceous adsorbed species. The heats of adsorption of the LFe° CO species on a C-free iron surface (for adsorption temperature Ta < 456 K), linearly vary with its coverage from ELFe°(1)=79 kJ/molELFe°(1)=79 kJ/mol to ELFe°(0)=105 kJ/molELFe°(0)=105 kJ/mol at high and low coverages. For Ta > 456 K, the CO dissociation overlaps the CO adsorption equilibrium leading to a C-containing iron surface. The presence of carbonaceous species has no significant impact on the heat of adsorption of the LFe° species at high coverages whereas it increases significantly that at low coverages: ELFe°(0)=120 kJ/mol.ELFe°(0)=120 kJ/mol. Considering reduced iron supported catalysts, the AEIR method is particularly useful because it allows the determination of the individual heats of adsorption of two adsorbed CO species that can be simultaneously present on the surface for high iron loadings. The study confirms that quantitative exploitations of DRIFT spectra are available for well designed experimental conditions offering an alternative for solid catalysts with low IR transmission properties.

Graphical abstractFigure optionsDownload full-size imageDownload high-quality image (226 K)Download as PowerPoint slideHighlights► Quantitative studies using diffuse reflectance mode. ► Adsorption equilibrium infrared spectroscopy method using DRIFT. ► Heat of adsorption of linear CO species on Fe2+ and Fe° sites of Fe/Al2O3. ► Impact of Cads species from the CO dissociation on the adsorbed CO species.

Keywords
Quantitative DRIFT; AEIR method; CO adsorption; Iron catalysts; Heats of adsorption
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Heats of adsorption of linear CO species adsorbed on reduced Fe/Al2O3 catalysts using the AEIR method in diffuse reflectance mode
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volumes 409–410, 15 December 2011, Pages 28–38
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
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Any Questions? feel free to contact us