期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 113, 期 32, 页码 8921-8926出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1605649113
关键词
single-atom catalysis; adsorbate induced sintering; redispersion; Fe3O4; nucleation and growth
资金
- Austrian Science Fund (FWF) [Y 847-N20, P24925-N20]
- Vienna University of Technology
- FWF, doctoral college SOLIDS4FUN [W1243]
- NWO-Vici [724.012.001]
- European Research Council (Advanced Grant OxideSurfaces)
- FWF [W1243, SFB F45, SFB F41]
- Austrian Science Fund (FWF) [P 24925] Funding Source: researchfish
- Austrian Science Fund (FWF) [W1243, P24925] Funding Source: Austrian Science Fund (FWF)
Interactions between catalytically active metal particles and reactant gases depend strongly on the particle size, particularly in the subnanometer regime where the addition of just one atom can induce substantial changes in stability, morphology, and reactivity. Here, time-lapse scanning tunneling microscopy (STM) and density functional theory (DFT)-based calculations are used to study how CO exposure affects the stability of Pt adatoms and subnano clusters at the Fe3O4(001) surface, a model CO oxidation catalyst. The results reveal that CO plays a dual role: first, it induces mobility among otherwise stable Pt adatoms through the formation of Pt carbonyls (Pt-1-CO), leading to agglomeration into subnano clusters. Second, the presence of the CO stabilizes the smallest clusters against decay at room temperature, significantly modifying the growth kinetics. At elevated temperatures, CO desorption results in a partial redispersion and recovery of the Pt adatom phase.
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