The Partial Oxidation of Methane Over Pd/Al2O3 Catalyst Nanoparticles Studied In-Situ by Near Ambient-Pressure X-ray Photoelectron Spectroscopy

• Published in: Topics in catalysis 2016-03, Vol.59 (5-7), p.516-525
• Main Authors: Price, Rachel, Eralp-Erden, Tuǧçe, Crumlin, Ethan, Rani, Sana, Garcia, Sonia, Smith, Richard, Deacon, Liam, Euaruksakul, Chanan, Held, Georg
• Format: Article
• Language: English
• Subjects: Catalysis; Characterization and Evaluation of Materials; Chemistry; Chemistry and Materials Science; Industrial Chemistry/Chemical Engineering; Original Paper; Pharmacy; Physical Chemistry
• ISSN: 1022-5528; 1572-9028
• DOI: 10.1007/s11244-015-0520-8

Near ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) is used to study the chemical state of methane oxidation catalysts in-situ. Al 2 O 3 –supported Pd catalysts are prepared with different particle sizes ranging from 4 to 10 nm. These catalysts were exposed to conditions similar to those used in the partial oxidation of methane (POM) to syn-gas and simultaneously monitored by NAP-XPS and mass spectrometry. NAP-XPS data show changes in the oxidation state of the palladium as the temperature increases, from metallic Pd 0 to PdO, and back to Pd 0 . Mass spectrometry shows an increase in CO production whilst the Pd is in the oxide phase, and the metal is reduced back under presence of newly formed H 2 . A particle size effect is observed, such that CH 4 conversion starts at lower temperatures with larger sized particles from 6 to 10 nm. We find that all nanoparticles begin CH 4 conversion at lower temperatures than polycrystalline Pd foil.