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

Journal Article · Mon Jul 09 00:00:00 EDT 2018 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1800262115· OSTI ID:1459485

He, Yang ^[1]; Liu, Jin-Cheng ^[2]; Luo, Langli ^[3]; Wang, Yang-Gang ^[2]; Zhu, Junfa ^[4]; Du, Yingge ^[5]; Li, Jun ^[6]; Mao, Scott X. ^[1]; Wang, Chongmin ^[3]

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1. Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, PA 15261,
2. Department of Chemistry, Tsinghua University, Beijing 100084, China,, Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education, Tsinghua University, Beijing 100084, China,
3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354,
4. National Synchrotron Radiation Laboratory, University of Science and Technology China, Hefei, Anhui 230029, China,, Department of Chemical Physics, University of Science and Technology China, Hefei, Anhui 230029, China,
5. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354
6. Department of Chemistry, Tsinghua University, Beijing 100084, China,, Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education, Tsinghua University, Beijing 100084, China,, Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99354,

Significance Gold is the noblest metal. However, when the size decreases to nanoscale and is supported on reducible oxides, the gold nanoparticle shows exceptionally high catalytic performance even at low temperatures. Here, through state-of-the-art in situ aberration-corrected environmental transmission electron microscopy and ab initio molecular-dynamic simulations, we discovered that, upon exposing to reactant gas (carbon monoxide and oxygen), ultrasmall gold clusters on ceria show a size-dependent order-to-disorder transformation with generation of dynamic low-coordinated atoms, which presumably can effectively boost the oxidation reaction of carbon monoxide. The findings provide much-needed insights on the origin of size-dependent catalytic properties of supported gold and demonstrate a size effect in absorbent–particle interactions that may widely exist and play an essential role in heterogeneous catalysts.

• Sponsoring Organization: USDOE
• Grant/Contract Number: 68278
• OSTI ID: 1459485
• Journal Information: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 115 Journal Issue: 30; ISSN 0027-8424
• Publisher: Proceedings of the National Academy of Sciences
• Country of Publication: United States
• Language: English