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Research Article

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

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.

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Graphical Abstract

In the case of catalysts where well-defined-shaped carriers are used as supports, when the size of the carrier approaches that of the loaded nanoparticles, the probability of contact between the nanoparticles and the edges of the carrier increases significantly. This leads to the formation of “edge-interfaces” that are different from the typical interface sites.

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

ceriananorodsupported catalystedge-effectatomic scale

Electronic Supplementary Material

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Nano Research
Volume 17 Issue 6,
June 2024
Pages 4986-4993
DOI: 10.1007/s12274-024-6508-6
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, 17(6): 4986-4993. https://doi.org/10.1007/s12274-024-6508-6
Topics:
Cerium oxideCrystal orientationHigh resolution transmission electron microscopyNanocatalysts

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Received: 17 November 2023
Revised: 06 January 2024
Accepted: 21 January 2024
Published: 23 March 2024
© Tsinghua University Press 2024
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