Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition

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 usi...

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Published inProceedings of the National Academy of Sciences - PNAS Vol. 115; no. 30; pp. 7700 - 7705
Main Authors He, Yang, Liu, Jin-Cheng, Luo, Langli, Wang, Yang-Gang, Zhu, Junfa, Du, Yingge, Li, Jun, 李隽, Mao, Scott X., Wang, Chongmin
Format Journal Article
LanguageEnglish
Published United States National Academy of Sciences 24.07.2018
Proceedings of the National Academy of Sciences
Subjects
Atoms & subatomic particles
Catalysis
Catalysts
Cerium oxides
Clusters
Cobalt
Gold
Molecular dynamics
Molecular structure
Nanoparticles
Oxidation
Physical Sciences
Size effects
Transmission electron microscopy
adsorbate-induced disorder
gold catalysis
dynamic low-coordinated atoms
size effect
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Summary: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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content type line 23
USDOE
68278
1Y.H., J.-C.L., and L.L. contributed equally to this work.
Edited by Catherine J. Murphy, University of Illinois at Urbana–Champaign, Urbana, IL, and approved June 12, 2018 (received for review January 5, 2018)
Author contributions: J.L., S.X.M., and C.W. designed research; Y.H., J.-C.L., L.L., Y.-G.W., J.Z., and Y.D. performed research; Y.H., J.-C.L., and L.L. analyzed data; and Y.H., J.-C.L., J.L., S.X.M., and C.W. wrote the paper.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1800262115