4.8 Article

Exceptional Activity for Methane Combustion over Modular Pd@CeO2 Subunits on Functionalized Al2O3

Journal

SCIENCE
Volume 337, Issue 6095, Pages 713-717

Publisher

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1222887

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Funding

  1. University of Trieste through FRA
  2. Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali (INSTM)
  3. Air Force Office of Scientific Research (Multidisciplinary University Research Initiative) [FA9550-08-1-0309]
  4. Ministry of Science and Innovation of Spain [CSD2009-00013]

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There is a critical need for improved methane-oxidation catalysts to both reduce emissions of methane, a greenhouse gas, and improve the performance of gas turbines. However, materials that are currently available either have low activity below 400 degrees C or are unstable at higher temperatures. Here, we describe a supramolecular approach in which single units composed of a palladium (Pd) core and a ceria (CeO2) shell are preorganized in solution and then homogeneously deposited onto a modified hydrophobic alumina. Electron microscopy and other structural methods revealed that the Pd cores remained isolated even after heating the catalyst to 850 degrees C. Enhanced metal-support interactions led to exceptionally high methane oxidation, with complete conversion below 400 degrees C and outstanding thermal stability under demanding conditions.

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