Journal Article FZJ-2015-03218

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Water-Gas Shift and Methane Reactivity on Reducible Perovskite-Type Oxides

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2015
Soc. Washington, DC

The journal of physical chemistry <Washington, DC> / C 119(21), 11739 - 11753 () [10.1021/acs.jpcc.5b02947]

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Abstract: Comparative (electro)catalytic, structural, and spectroscopic studies in hydrogen electro-oxidation, the (inverse) water-gas shift reaction, and methane conversion on two representative mixed ionic–electronic conducting perovskite-type materials La0.6Sr0.4FeO3−δ (LSF) and SrTi0.7Fe0.3O3−δ (STF) were performed with the aim of eventually correlating (electro)catalytic activity and associated structural changes and to highlight intrinsic reactivity characteristics as a function of the reduction state. Starting from a strongly prereduced (vacancy-rich) initial state, only (inverse) water-gas shift activity has been observed on both materials beyond ca. 450 °C but no catalytic methane reforming or methane decomposition reactivity up to 600 °C. In contrast, when starting from the fully oxidized state, total methane oxidation to CO2 was observed on both materials. The catalytic performance of both perovskite-type oxides is thus strongly dependent on the degree/depth of reduction, on the associated reactivity of the remaining lattice oxygen, and on the reduction-induced oxygen vacancies. The latter are clearly more reactive toward water on LSF, and this higher reactivity is linked to the superior electrocatalytic performance of LSF in hydrogen oxidation. Combined electron microscopy, X-ray diffraction, and Raman measurements in turn also revealed altered surface and bulk structures and reactivities.

Classification:

Contributing Institute(s):
  1. Mikrostrukturforschung (PGI-5)
Research Program(s):
  1. 143 - Controlling Configuration-Based Phenomena (POF3-143) (POF3-143)

Appears in the scientific report 2015
Database coverage:
Medline ; Creative Commons Attribution CC BY 3.0 ; OpenAccess ; Current Contents - Physical, Chemical and Earth Sciences ; IF < 5 ; JCR ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection
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 Record created 2015-05-20, last modified 2024-06-10