The role of chromium in iron-based high-temperature water-gas shift catalysts under industrial conditions

M. I. Ariëns, V. Chlan, P. Novák, L. G.A. van de Water, A. I. Dugulan, E. Brück, E. J.M. Hensen

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Abstract

Chromium promotion of iron oxide based water-gas shift (WGS) catalysts prepared via co-precipitation/calcination was investigated. Mössbauer spectroscopy and XRD evidence that chromium is incorporated in the calcined hematite (α-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. Mössbauer 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 Mössbauer 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.

Original languageEnglish
Article number120465
Number of pages14
JournalApplied Catalysis B: Environmental
Volume297
DOIs
Publication statusPublished - 2021

Keywords

  • Chromium
  • Iron oxide
  • Mössbauer spectroscopy
  • Promotion
  • Water-gas shift reaction

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