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Research Article | Online first | Published: 23 March 2024

Geometric edge effect on the interface of Au/CeO2 nanocatalysts for CO oxidation

Show Author's Information Hongpeng Liu1,§,  Zhongliang Cao1,§,  Siyuan Yang1,§,  Qingye Ren1,  Zejian Dong1,  Wei Liu2,  Zi-An Li3( ),  Xing Chen1,4( ),  Langli Luo1,4( )
Institute of Molecular Plus, Tianjin University, Tianjin 300072, China
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics (DICP), Chinese Academy of Sciences, Dalian 116023, China
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, and School of Physical Science and Technology, Guangxi University, Nanning 530004, China
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China

§ Hongpeng Liu, Zhongliang Cao, and Siyuan Yang contributed equally to this work.

Keywords:
ceria, supported catalyst, nanorod, atomic scale, edge-effect
Topics:
Cerium oxideCrystal orientationHigh resolution transmission electron microscopyNanocatalysts
Cite this article:
Liu H, Cao Z, Yang S, et al. Geometric edge effect on the interface of Au/CeO2 nanocatalysts for CO oxidation. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6508-6
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Abstract Full text Electronic supplementary material About this article

The oxide supports play a crucial role in anchoring and promoting the active metal species by geometric confinement and chemical interaction. The design and synthesis of the well-defined oxide support with specific morphology such as size, shape, and exposed facets have attracted extensive research efforts, which directly reflects on their catalytic performance. In this study, using an Au/CeO2-nanorod model catalyst, we demonstrate an edge effect on the Au/CeO2 interfacial structure, which shows a prominent effect on the structure–performance relationship in the CO oxidation reaction. This specific “edge-interface” structure features an “edge-on” Au nanoparticles position on rod-shaped CeO2 support, confirmed by atomic-scale electron microscopy characterization, which introduces additional degrees of freedom in coordination environment, chemical state, bond length, and strength. Combined with theocratical calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) investigations, we confirmed that this “edge-interface” has distinct adsorption properties due to the change of O vacancy formation energy as well as the chemical states of Au resulting from the electron transfer and redistribution between the metal and the support. These results demonstrate a non-conventional geometric effect of rod-shaped supported metal catalysts on the catalytic performance, which could provide insights into the atomic-precise utilization of catalysts.


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About this article

Geometric edge effect on the interface of Au/CeO2 nanocatalysts for CO oxidation

Show Author's information Hongpeng Liu1,§, Zhongliang Cao1,§, Siyuan Yang1,§, Qingye Ren1, Zejian Dong1, Wei Liu2, Zi-An Li3( ), Xing Chen1,4( ), Langli Luo1,4( )
Institute of Molecular Plus, Tianjin University, Tianjin 300072, China
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics (DICP), Chinese Academy of Sciences, Dalian 116023, China
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, and School of Physical Science and Technology, Guangxi University, Nanning 530004, China
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China

§ Hongpeng Liu, Zhongliang Cao, and Siyuan Yang contributed equally to this work.

Abstract

The oxide supports play a crucial role in anchoring and promoting the active metal species by geometric confinement and chemical interaction. The design and synthesis of the well-defined oxide support with specific morphology such as size, shape, and exposed facets have attracted extensive research efforts, which directly reflects on their catalytic performance. In this study, using an Au/CeO2-nanorod model catalyst, we demonstrate an edge effect on the Au/CeO2 interfacial structure, which shows a prominent effect on the structure–performance relationship in the CO oxidation reaction. This specific “edge-interface” structure features an “edge-on” Au nanoparticles position on rod-shaped CeO2 support, confirmed by atomic-scale electron microscopy characterization, which introduces additional degrees of freedom in coordination environment, chemical state, bond length, and strength. Combined with theocratical calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) investigations, we confirmed that this “edge-interface” has distinct adsorption properties due to the change of O vacancy formation energy as well as the chemical states of Au resulting from the electron transfer and redistribution between the metal and the support. These results demonstrate a non-conventional geometric effect of rod-shaped supported metal catalysts on the catalytic performance, which could provide insights into the atomic-precise utilization of catalysts.

Keywords: ceria, supported catalyst, nanorod, atomic scale, edge-effect

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Acknowledgements

Publication history

Received: 17 November 2023
Revised: 06 January 2024
Accepted: 21 January 2024
Published: 23 March 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

The authors appreciate the support from the National Natural Science Foundation of China (Nos. 22172110 and 12364018) and the Guangxi Science and Technology Major Program (No. AA23073019). We thank the Haihe Laboratory of Sustainable Chemical Transformations for financial support. We thank the Facility Center at the Institute of Molecular Plus at Tianjin University, Facility and Analysis Center at Guangxi University, and Electron Microscopy Center at the Dalian Institute of Chemical Physics, Chinese Academy of Sciences to use the transmission electron microscopy.

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