4.7 Article

Catalytic properties of dispersed iron oxides Fe2O3/MO2 (M = Zr, Ce, Ti and Si) for sulfuric acid decomposition reaction: Role of support

期刊

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 43, 期 1, 页码 37-52

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PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2017.10.163

关键词

Supported iron oxide; Sulfuric acid decomposition; epsilon-Fe2O3; Metal oxide-support interaction; Thermochemical cycle; Hydrogen generation

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Supported iron oxides have been established as an important class of catalyst for high temperature sulfuric acid decomposition. With an objective to elucidate the role of support in modifying the overall catalytic properties of dispersed iron oxide catalysts, a series of supported iron oxide based catalysts, Fe2O3 (15 wt%)/MO2 (M = Zr, Ce, Ti and Si), synthesized by adsorption-equilibrium method, is investigated for sulfuric acid decomposition reaction. The structure of dispersed iron oxide phases largely depended on the nature of the support oxide as revealed by the XRD and Mossbauer studies. alpha-Fe2O3 is found to be present as a major phase on ZrO2 and CeO2 support while epsilon-Fe2O3 was the major phase on silica supported iron oxide. On the other hand, presence of mixed oxide Fe2TiO5 was revealed over TiO2 support. Strong dispersed metal oxide-support interactions inhibited the total reduction of the dispersed phase on SiO2 and TiO2 as compared to complete reduction of dispersed iron oxide on CeO2 and ZrO2 supports during temperature programmed reduction upto 1000 degrees C. The order of catalytic activity at a temperature of similar to 750 degrees C is observed as Fe2O3/SiO2 > Fe2TiO5/TiO2 > Fe2O3/ZrO2 > Fe2O3/CeO2, while at higher temperatures of similar to 900 degrees C the SO2 yield is found to be comparable for all catalysts. A relationship between the rate of sulfate decomposition and catalytic activity is established through detailed TG-DTA investigations of sulfated catalyst and support. Considerable influence of the support oxide on the composition, structure, redox properties, morphology and catalytic activities of the active iron oxide dispersed phase has been observed. Thus, the support oxides operate as a critical component in the complex supported metal oxide catalysts and these findings might influence the design and development of future high temperature sulfuric acid decomposition catalysts. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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