Defect Dynamics at a Single Pt Nanoparticle during Catalytic Oxidation

Abstract

Defects can affect all aspects of a material by altering its electronic properties and controlling its chemical reactivity. At defect sites, preferential adsorption of reactants and/or formation of chemical species at active sites are observed in heterogeneous catalysis. Understanding the structural response at defect sites during catalytic reactions provides a unique opportunity to exploit defect control of nanoparticle-based catalysts. However, it remains difficult to characterize the strain and defect evolution for a single nanocrystal catalyst in situ. Here, we report Bragg coherent X-ray diffraction imaging of defect dynamics in an individual Pt nanoparticle during catalytic methane oxidation. We observed that the initially tensile strained regions of the crystal became seed points for the development of further strain and subsequent disappearance of diffraction density during oxidation reactions. Our detailed understanding of the catalytically induced deformation at the defect sites and observed reversibility during the relevant steps of the catalytic oxidation process provide important insights of defect control and engineering of heterogeneous catalysts.