Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 30, Pages 7700-7705Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1800262115
Keywords
gold catalysis; size effect; adsorbate-induced disorder; dynamic low-coordinated atoms
Categories
Funding
- Laboratory Directed Research and Development program at Pacific Northwest National Laboratory (PNNL)
- US Department of Energy, Office of Biological and Environmental Research
- US Department of Energy [DE-AC05-76RLO1830]
- National Key Basic Research Special Foundation [2013CB834603]
- National Natural Science Foundation of China of China [91645203, 21521091, 21590792]
- National Science Foundation through University of Pittsburgh [CMMI 1536811]
- National Basic Research Program of China [2013CB834605]
- Scientific Research and Users with Potential Grants of Hefei Science Center of Chinese Academy of Sciences [2015SRG-HSC031, 2015HSC-UP022]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Early Career Research Program [68278]
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Gold (Au) catalysts exhibit a significant size effect, but its origin has been puzzling for a long time. It is generally believed that supported Au clusters are more or less rigid in working condition, which inevitably leads to the general speculation that the active sites are immobile. Here, by using atomic resolution in situ environmental transmission electron microscopy, we report size-dependent structure dynamics of single Au nanoparticles on ceria (CeO2) in CO oxidation reaction condition at room temperature. While large Au nanoparticles remain rigid in the catalytic working condition, ultrasmall Au clusters lose their intrinsic structures and become disordered, featuring vigorous structural rearrangements and formation of dynamic low-coordinated atoms on surface. Ab initio molecular-dynamics simulations reveal that the interaction between ultrasmall Au cluster and CO molecules leads to the dynamic structural responses, demonstrating that the shape of the catalytic particle under the working condition may totally differ from the shape under the static condition. The present observation provides insight on the origin of superior catalytic properties of ultrasmall gold clusters.
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