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1.
Chemphyschem ; 24(6): e202200648, 2023 Mar 14.
Artículo en Inglés | MEDLINE | ID: mdl-36380531

RESUMEN

We report on bimetallic FeRh clusters with a narrow size-distribution grown on graphene on Ir(111) as a carbon-supported model catalyst to promote low-temperature catalytic CO oxidation. By combining scanning tunneling microscopy with catalytic performance measurements, we reveal that Fe-Rh interfaces are active sites for oxygen activation and CO oxidation, especially at low temperatures. Rh core Fe shell clusters not only provide the active sites for the reaction, but also thermally stabilize surface Fe atoms towards coarsening compared with pure Fe clusters. Alternate isotope-labelled CO/O2 pulse experiments show opposite trends on preferential oxidation (PROX) performance because of surface hydroxyl species formation and competitive adsorption between CO and O2 . The present results introduce a general strategy to stabilize metallic clusters and to reveal the reaction mechanisms on bimetallic structures for low-temperature catalytic CO oxidation as well as preferential oxidation.

2.
Nano Lett ; 21(19): 8266-8273, 2021 Oct 13.
Artículo en Inglés | MEDLINE | ID: mdl-34569802

RESUMEN

Single atom magnets offer the possibility of magnetic information storage in the most fundamental unit of matter. Identifying the parameters that control the stability of their magnetic states is crucial to design novel quantum magnets with tailored properties. Here, we use X-ray absorption spectroscopy to show that the electronic configuration of dysprosium atoms on MgO(100) thin films can be tuned by the proximity of the metal Ag(100) substrate onto which the MgO films are grown. Increasing the MgO thickness from 2.5 to 9 monolayers induces a change in the dysprosium electronic configuration from 4f9 to 4f10. Hysteresis loops indicate long magnetic lifetimes for both configurations, however, with a different field-dependent magnetic stability. Combining these measurements with scanning tunneling microscopy, density functional theory, and multiplet calculations unveils the role of the adsorption site and charge transfer to the substrate in determining the stability of quantum states in dysprosium single atom magnets.

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