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Ethanol Steam Reforming: Higher Dehydrogenation Selectivities Observed by Tuning Oxygen-Mobility and Acid/Base Properties with Mn in CeO2·MnOx·SiO2 Catalysts

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Abstract

Doping CeO2–SiO2 catalysts with Mn was found to increase H2 selectivity and decrease ethylene selectivity. In the presence of SiO2, relatively high surface areas (~150–190 m2 g−1 range) were stabilized with these coprecipitated catalysts after calcining at 500 °C for 5 h. By means of a combination of ex-situ (XRD, TPR, CO2–TPD, OSC measurements) along with in situ (Ce LIII edge XANES, DRIFTS) techniques Mn was proposed to act to improve the ability of ceria to deliver active oxygen surface species essential to the stepwise oxidative dehydrogenation of adsorbed species from ethoxides to acetates. Doping ceria with Mn at low levels improved the carbonate decomposition rate by weakening surface basicity. At high Mn content, acetates become too stable and poison catalytically active sites.

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Acknowledgments

This work received financial support from CTENERG/FINEP-01.04.0525.00. CAER acknowledges the Commonwealth of Kentucky for financial support. M.C. Ribeiro acknowledges the scholarship received from CNPq. The group thanks the Laboratório Nacional de Luz Síncrotron for the opportunity to perform XANES measurements.

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Authors and Affiliations

  1. Instituto Nacional de Tecnologia, Av. Venezuela 82, Rio de Janeiro, RJ, CEP 20081-312, Brazil

    Mauro C. Ribeiro & Fábio B. Noronha

  2. Center for Applied Energy Research, The University of Kentucky, 2540 Research Park Drive, Lexington, KY, 40511, USA

    Gary Jacobs & Burtron H. Davis

  3. Universidade Federal Fluminense, Rua Passo da Pátria, 156, Niterói, RJ, CEP 24210-240, Brazil

    Lisiane V. Mattos

Authors
  1. Mauro C. Ribeiro
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  2. Gary Jacobs
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  3. Burtron H. Davis
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  4. Lisiane V. Mattos
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  5. Fábio B. Noronha
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Correspondence to Burtron H. Davis.

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Ribeiro, M.C., Jacobs, G., Davis, B.H. et al. Ethanol Steam Reforming: Higher Dehydrogenation Selectivities Observed by Tuning Oxygen-Mobility and Acid/Base Properties with Mn in CeO2·MnOx·SiO2 Catalysts. Top Catal 56, 1634–1643 (2013). https://doi.org/10.1007/s11244-013-0098-y

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  • DOI: https://doi.org/10.1007/s11244-013-0098-y

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