4.8 Article

Outstanding Methane Oxidation Performance of Palladium-Embedded Ceria Catalysts Prepared by a One-Step Dry Ball-Milling Method

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 32, Pages 10212-10216

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201805929

Keywords

ceria; combustion; mechanochemistry; methane; palladium

Funding

  1. Ford Motor Company [2014-2195R]
  2. Regione Friuli Venezia Giulia under Operating Program of the European Social Fund 2014/2020
  3. MINECO/FEDER [ENE2015-63969, GC 2017 SGR 128]

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By carefully mixing Pd metal nanoparticles with CeO2 polycrystalline powder under dry conditions, an unpredicted arrangement of the Pd-O-Ce interface is obtained in which an amorphous shell containing palladium species dissolved in ceria is covering a core of CeO2 particles. The robust contact that is generated at the nanoscale, along with mechanical forces generated during mixing, promotes the redox exchange between Pd and CeO2 and creates highly reactive and stable sites constituted by PdOx embedded into CeO2 surface layers. This specific arrangement outperforms conventional Pd/CeO2 reference catalysts in methane oxidation by lowering light-off temperature by more than 50 degrees C and boosting the reaction rate. The origin of the outstanding activity is traced to the structural properties of the interface, modified at the nanoscale by mechanochemical interaction.

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