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Issue 6, 2011
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Regenerable Fe–Mn–ZnO/SiO2 sorbents for room temperature removal of H2S from fuel reformates: performance, active sites, Operando studies

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Abstract

Fe- and Mn-promoted H2S sorbents Fex–Mny–Zn1−xyO/SiO2 (x, y = 0, 0.025) for desulfurization of model fuel reformates at room temperature were prepared, tested and characterized. Sulfur uptake capacity at 25 °C significantly exceeds that of both commercial unsupported ZnO sorbents and un-promoted supported ZnO/SiO2 sorbents. Sulfur capacity and breakthrough characteristics remain satisfactory after multiple (∼10) cycles of adsorption/regeneration, with regeneration performed by a simple and robust heating in air. XRD shows that both “calcined” and “spent” sorbents contain nano-dispersed ZnO, and XPS confirms conversion of ZnO to ZnS. “Calcined” sorbent contains Fe3+ and Mn3+ that are reduced to Mn2+ upon reaction with H2S, but not with H2. Operando ESR is used for the first time to study dynamics of reduction of Mn3+ promoter sites simultaneously with measuring sulfidation dynamics of the Fex–Mny–Zn1−xyO/SiO2 sorbent. Fe cations are believed to occupy the surface of supported ZnO nanocrystallites, while Mn cations are distributed within ZnO.

Graphical abstract: Regenerable Fe–Mn–ZnO/SiO2 sorbents for room temperature removal of H2S from fuel reformates: performance, active sites, Operando studies

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Publication details

The article was received on 28 Jul 2010, accepted on 04 Nov 2010 and first published on 06 Dec 2010


Article type: Paper
DOI: 10.1039/C0CP01355B
Citation: Phys. Chem. Chem. Phys., 2011,13, 2179-2187
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    Regenerable Fe–Mn–ZnO/SiO2 sorbents for room temperature removal of H2S from fuel reformates: performance, active sites, Operando studies

    P. Dhage, A. Samokhvalov, D. Repala, E. C. Duin and B. J. Tatarchuk, Phys. Chem. Chem. Phys., 2011, 13, 2179
    DOI: 10.1039/C0CP01355B

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