Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 297, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120465
Keywords
Water-gas shift reaction; Iron oxide; Chromium; Promotion; Mossbauer spectroscopy
Funding
- Dutch Research Council (NWO) [731.015.419]
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Research has shown that chromium enhances the water-gas shift activity of iron oxide catalysts, leading to increased CO conversion rates by preventing the reduction of Fe3+ to Fe2+. Despite an increase in the Fe3+/Fe2+ ratio, the presence of chromium does not affect the high CO conversion rates associated with structural stabilization mechanisms.
Chromium promotion of iron oxide based water-gas shift (WGS) catalysts prepared via co-precipitation/calcination was investigated. Mossbauer spectroscopy and XRD evidence that chromium is incorporated in the calcined hematite (alpha-Fe2O3) precursor irrespective of the doping level (0-12 wt.%). CO-TPR shows chromium delays the reduction of hematite and the active magnetite (Fe3O4) phase. WGS activity was evaluated under realistic conditions for 4 days. Enhanced CO conversion was observed with increased chromium doping. Mossbauer spectra indicate that chromium incorporates into octahedral sites of magnetite and prevents reduction of Fe3+ to Fe2+ during formation of the active phase, leading to an increased Fe3+/Fe2+ ratio in octahedral sites. The higher Fe3+/Fe2+ ratio did not affect the high CO conversion associated with the structural stabilization mechanism of Cr-doping. Interpretation of the Mossbauer spectra was supported by computational modelling of various chromium and vacancy-doped magnetite structures. The bulk structure of an in situ prepared chromium-doped high-temperature WGS catalyst is best described as a partially oxidized chromium-doped magnetite phase. No surface effects of Cr-doping were found.
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