The Active Phase of Palladium during Methane Oxidation
- 23 February 2012
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry Letters
- Vol. 3 (6), 678-682
- https://doi.org/10.1021/jz300069s
Abstract
The active phase of Pd during methane oxidation is a long-standing puzzle, which, if solved, could provide routes for design of improved catalysts. Here, density functional theory and in situ surface X-ray diffraction are used to identify and characterize atomic sites yielding high methane conversion. Calculations are performed for methane dissociation over a range of Pd and PdOx surfaces and reveal facile dissociation on either under-coordinated Pd sites in PdO(101) or metallic surfaces. The experiments show unambiguously that high methane conversion requires sufficiently thick PdO(101) films or metallic Pd, in full agreement with the calculations. The established link between high activity and atomic structure enables rational design of improved catalysts.Keywords
This publication has 34 references indexed in Scilit:
- Surface structure and reactivity of Pd(100) during CO oxidation near ambient pressuresPhysical Chemistry Chemical Physics, 2011
- CO Oxidation on Technological Pd−Al2O3Catalysts: Oxidation State and ActivityThe Journal of Physical Chemistry C, 2010
- Ultrahigh vacuum/high-pressure flow reactor for surface x-ray diffraction and grazing incidence small angle x-ray scattering studies close to conditions for industrial catalysisReview of Scientific Instruments, 2010
- The ID03 surface diffraction beamline for in-situ and real-time X-ray investigations of catalytic reactions at surfacesCatalysis Today, 2009
- CO oxidation trends on Pt-group metals from ultrahigh vacuum to near atmospheric pressures: A combined in situ PM-IRAS and reaction kinetics studySurface Science, 2008
- oxidation at: A first-principles constrained thermodynamics studyPhysical Review B, 2007
- Thermodynamic stability of PdO surfacesPhysical Review B, 2004
- Kinetics of PdO combustion catalysisCatalysis Today, 1995
- Surface diffraction beamline at ESRFReview of Scientific Instruments, 1995
- Projector augmented-wave methodPhysical Review B, 1994