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arxiv 2103.01573 v1 pith:QEL53COE submitted 2021-03-02 cond-mat.mtrl-sci cond-mat.mes-hall

Single Alloy Nanoparticle X-Ray Imaging during a Catalytic Reaction

classification cond-mat.mtrl-sci cond-mat.mes-hall
keywords facetreactionundercompositionconditionsimagingnanoparticlestrain
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts dynamics. We report the facet resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment dependent chemical composition. We find that the initially Pt terminated nanoparticle surface gets Rh enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent and the Rh enrichment is non-reversible under subsequent CO reduction. Tracking facet resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity and lifetime.

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