Tracking the shape-dependent sintering of platinum–rhodium model catalysts under operando conditions

Uta Hejral, Patrick Müller, Olivier Balmes, Diego Pontoni and Andreas Stierle ()
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Uta Hejral: Deutsches Elektronen-Synchrotron (DESY), NanoLab
Patrick Müller: Deutsches Elektronen-Synchrotron (DESY), NanoLab
Olivier Balmes: MAX IV Laboratory
Diego Pontoni: ESRF - The European Synchrotron, Radiation Facility
Andreas Stierle: Deutsches Elektronen-Synchrotron (DESY), NanoLab

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: Abstract Nanoparticle sintering during catalytic reactions is a major cause for catalyst deactivation. Understanding its atomic-scale processes and finding strategies to reduce it is of paramount scientific and economic interest. Here, we report on the composition-dependent three-dimensional restructuring of epitaxial platinum–rhodium alloy nanoparticles on alumina during carbon monoxide oxidation at 550 K and near-atmospheric pressures employing in situ high-energy grazing incidence x-ray diffraction, online mass spectrometry and a combinatorial sample design. For platinum-rich particles our results disclose a dramatic reaction-induced height increase, accompanied by a corresponding reduction of the total particle surface coverage. We find this restructuring to be progressively reduced for particles with increasing rhodium composition. We explain our observations by a carbon monoxide oxidation promoted non-classical Ostwald ripening process during which smaller particles are destabilized by the heat of reaction. Its driving force lies in the initial particle shape which features for platinum-rich particles a kinetically stabilized, low aspect ratio.

Date: 2016
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DOI: 10.1038/ncomms10964

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