460805 Promotion Mechanisms of Iron Oxide-Based High Temperature-Water Gas Shift (HT-WGS) Catalysts By Chromium and Copper

Thursday, November 17, 2016: 10:10 AM
Franciscan B (Hilton San Francisco Union Square)
Tulio Rocha1, Minghui Zhu2, Axel Knop-Gericke3, Israel Wachs4 and Robert Schlogl1, (1)Inorganic Chemistry, Fritz Haber Institute of the Max Planck Society, Berlin, Germany, (2)Chemical Engineering, Lehigh University, Bethlehem, PA, (3)Inorganic Chemistry, Fritz Haber Institute of the Max Planck Society, Berlin, Germany, Fritz Haber Institute of the Max Planck Society, (4)Chemical and Biomolecular Engineering, Lehigh University, Bethlehem, PA

The Cr and Cu promotion mechanisms of high temperature water-gas shift (HT-WGS) iron oxide catalysts, synthesized by co-precipitation, were investigated as a function of reaction conditions. XRD and in situ Raman characterization showed that the initial calcined catalysts consisted of the Fe2O3 (hematite) bulk phase and transformed to the Fe3O4 (magnetite) phase during the HT-WGS reactions. In situ NAP-XPS and HS-LEIS surface analysis revealed that Cr was surface enriched as Cr+6 for the initial catalyst and reduced to Cr+3 during the HT-WGS reactions, with the Cr+3 dissolving into the bulk iron oxide lattice forming a solid solution. In situ NAP-XPS, XANES and HS-LEIS characterization indicated that Cu was initially present as Cu+2 cations dissolved in the Fe2O3 bulk lattice and reduced to metallic Cu0 nanoparticles (~3nm) on the external surface of the iron oxide support during the HT-WGS reactions. In situ HS-LEIS surface analysis also suggests that ~1/3 of the surface of the Cu nanoparticles was covered by a FeOx overlayer. The CO-TPR probe demonstrated that Cr does not chemically promote the iron oxide catalyst and that only Cu is a chemical promoter for the iron oxide HT-WGS catalysts. The Cu promoter introduces new catalytic active sites that enhance the reaction rates of the WGS reactions.

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