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Planar and tubular perovskite-type membrane reactors for the partial oxidation of methane to syngas

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Abstract

Dense planar and tubular oxygen separation membranes of La0.6Ca0.4Fe0.75Co0.25O3−δ were investigated as reactors for the partial oxidation (POX) of methane to syngas. Their permeation properties were measured in an air/argon pO2 gradient as a function of temperature. At 900 °C, the oxygen flux through a 1.26-mm-thick membrane was 0.075 μmol/cm2·s and through a 0.25-mm-thick tube, 0.24 μmol/cm2·s.

For the POX measurements, a catalyst was added to the membrane and methane was introduced on the argon side. This resulted in a gradual increase of the oxygen flux with increasing concentration of methane, reaching 2 μmol/cm2·s at 900 °C with pure methane. For the planar reactor, the CO selectivity reached 99% and the CH4 conversion 75% at 918 °C with pure methane. For the tubular reactor, the CO selectivity and CH4 conversion were 83 and 99%, respectively, under the same conditions. After 1,400 h of operation in a tubular POX reactor, the membrane was examined revealing phase demixing and local decomposition.

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Acknowledgements

This work was supported by the Swiss Natural Gas Union Funding (FOGA). H. Schindler, from EMPA-Dübendorf, produced the powder.

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Authors and Affiliations

  1. Laboratory for Industrial Energy Systems (LENI), STI, Swiss Federal Institute of Technology, 1015, Lausanne, Switzerland

    Stefan Diethelm, Jan Van herle & Daniel Favrat

  2. HTceramix, EPFL Science Park, PSE-A, 1015, Lausanne, Switzerland

    Joseph Sfeir

  3. Swiss Federal Laboratory for Materials Testing and Research (EMPA), 8600, Dübendorf, Switzerland

    Frank Clemens

Authors
  1. Stefan Diethelm
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  2. Joseph Sfeir
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  3. Frank Clemens
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  4. Jan Van herle
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  5. Daniel Favrat
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Corresponding author

Correspondence to Stefan Diethelm.

Additional information

Presented at the OSSEP Workshop “Ionic and Mixed Conductors: Methods and Processes”, Aveiro, Portugal, 10–12 April 2003

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Diethelm, S., Sfeir, J., Clemens, F. et al. Planar and tubular perovskite-type membrane reactors for the partial oxidation of methane to syngas. J Solid State Electrochem 8, 611–617 (2004). https://doi.org/10.1007/s10008-003-0489-2

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  • DOI: https://doi.org/10.1007/s10008-003-0489-2

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