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Catalytic CO Oxidation over Au Nanoparticles Supported on CeO2 Nanocrystals: Effect of the Au–CeO2 Interface
Abstract
Gold nanoparticles (NPs) have attracted attention due to their superior catalytic performance in CO oxidation at low temperatures. Along with the size and shape of Au NPs, the catalytic function of Au-catalyzed CO oxidation can be further optimized by controlling the physicochemical properties of oxide-supporting materials. We applied a combinatorial approach of experimental analyses and theoretical interpretations to study the effect of a surface structure of supporting oxides and the corresponding CO oxidation activity of supported Au NPs. We synthesized Au NPs (average d ≈ 3 nm) supported on shape-controlled CeO 2 nanocrystals, Au/CeO 2 cubes, and Au/CeO 2 octahedra for experimental analyses. The catalysts were modeled as Au/CeO 2 (100) and Au/CeO 2 (111) via density functional theory (DFT) calculations. The DFT calculations showed that the O–C–O type reaction intermediate could be spontaneously formed at the Au–CeO 2 (100) interface upon sequential multi-CO adsorption, accelerating CO oxidation via the Mars-van Krevelen mechanism. The additional kinetic process required for O–C–O formation at the Au–CeO 2 (111) interface slowed down the reaction. The experimental turnover frequency (TOF) of the Au/CeO 2 cubes was 4 times greater than that of the Au/CeO 2 octahedra (under 0.05 bar CO and 0.13 bar O 2 ). The increasing TOF as a function of CO partial pressure and the positive correlation between the reducibility of CeO 2 and the catalytic activity of Au/CeO 2 catalysts confirmed the theoretical prediction that CO molecules occupy the surface of Au NPs and that the oxidation of Au-bound CO occurs at the Au–CeO 2 interface. Through a comparative study of DFT calculations and in-depth experimental analyses, we provide insights into the catalytic function of CeO 2 -supported Au NPs toward CO oxidation depending on the shape of CeO 2 and ratio of CO/O 2 .
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Cites
Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
Tauster, S. J., Fung, S. C., & Garten, R. L. (1978) · Journal of the American Chemical Society · doi:10.1021/ja00469a029 · Cited by 3,188
Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation
Herzing, A. A., Kiely, C. J., Carley, A. F., Landon, P., & Hutchings, G. J. (2008) · Science · doi:10.1126/science.1159639 · Cited by 1,530
Cited by
Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity
van Deelen, T. W., Hernández Mejía, C., & de Jong, K. P. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0364-x · Cited by 2,349
Metal–support interactions in metal oxide-supported atomic, cluster, and nanoparticle catalysis
Leybo, D., Etim, U. J., Monai, M., Bare, S. R., Zhong, Z., & Vogt, C. (2024) · Chemical Society Reviews · doi:10.1039/d4cs00527a · Cited by 417
He, S., Yan, C., Chen, X.-Z., Wang, Z., Ouyang, T., Guo, M.-L., & Liu, Z.-Q. (2020) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2020.119138 · Cited by 281
Metadata
- Authors
- Ha, H., Yoon, S., An, K., & Kim, H. Y.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-10-25
- Volume
- 8
- Issue
- 12
- Pages
- 11491-11501
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2898382697
- Cited by
- 242
- References
- 2
- FWCI
- 9.13
- Type
- journal article
- Language
- en
- Open access
- closed
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