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

Abstract

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 (CeO 2 ) 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.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1459485
Grant/Contract Number:  
68278
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 30; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

He, Yang, Liu, Jin-Cheng, Luo, Langli, Wang, Yang-Gang, Zhu, Junfa, Du, Yingge, Li, Jun, Mao, Scott X., and Wang, Chongmin. Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition. United States: N. p., 2018. Web. doi:10.1073/pnas.1800262115.
He, Yang, Liu, Jin-Cheng, Luo, Langli, Wang, Yang-Gang, Zhu, Junfa, Du, Yingge, Li, Jun, Mao, Scott X., & Wang, Chongmin. Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition. United States. doi:10.1073/pnas.1800262115.
He, Yang, Liu, Jin-Cheng, Luo, Langli, Wang, Yang-Gang, Zhu, Junfa, Du, Yingge, Li, Jun, Mao, Scott X., and Wang, Chongmin. Mon . "Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition". United States. doi:10.1073/pnas.1800262115.
@article{osti_1459485,
title = {Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition},
author = {He, Yang and Liu, Jin-Cheng and Luo, Langli and Wang, Yang-Gang and Zhu, Junfa and Du, Yingge and Li, Jun and Mao, Scott X. and Wang, Chongmin},
abstractNote = {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 (CeO 2 ) 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.},
doi = {10.1073/pnas.1800262115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 30,
volume = 115,
place = {United States},
year = {2018},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1073/pnas.1800262115

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Cited by: 12 works
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