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

Literature Information

Publication Date 2010-12-06
DOI 10.1039/C0CP01355B
Impact Factor 3.676
Authors

Priyanka Dhage, Divya Repala, Evert C. Duin, Bruce J. Tatarchuk


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Abstract

Fe- and Mn-promoted H2S sorbents Fex–Mny–Zn1−x−yO/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−x−yO/SiO2 sorbent. Fe cations are believed to occupy the surface of supported ZnO nanocrystallites, while Mn cations are distributed within ZnO.

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