Citation: WANG Yan, LI Xiong, HU Shanwei, XU Qian, JU Huanxin, ZHU Junfa. Morphologies and Electronic Structures of Calcium-Doped Ceria Model Catalysts and Their Interaction with CO₂[J]. Acta Physico-Chimica Sinica, ;2018, 34(12): 1381-1389. doi: 10.3866/PKU.WHXB201804092 shu

Morphologies and Electronic Structures of Calcium-Doped Ceria Model Catalysts and Their Interaction with CO₂

National Synchrotron Radiation Laboratory, Department of Chemical Physics, University of Science and Technology of China, Hefei 230029, P. R. China

Corresponding author: HU Shanwei, husw@ustc.edu.cn ZHU Junfa, jfzhu@ustc.edu.cn
Received Date: 14 March 2018
Revised Date: 2 April 2018
Accepted Date: 3 April 2018
Available Online: 9 December 2018
Fund Project: China Postdoctoral Science Foundation BH2310000032The project was supported by the National Natural Science Foundation of China 21403205National Key Technologies R & D Program of China 2017YFA0403402The project was supported by the National Natural Science Foundation of China (U1732272, 21473178, 21403205), National Key Technologies R & D Program of China (2017YFA0403402), and China Postdoctoral Science Foundation (BH2310000032)The project was supported by the National Natural Science Foundation of China 21473178The project was supported by the National Natural Science Foundation of China U1732272

CeO₂-based catalysts are promising for use in various important chemical reactions involving CO₂, such as the dry reforming of methane to produce synthesis gas and methanol. CeO₂ has a superior ability to store and release oxygen, which can improve the catalytic performance by suppressing the formation of coke. Although the adsorption and activation behavior of CO₂ on the CeO₂ surface has been extensively investigated in recent years, the intermediate species formed from CO₂ on ceria has not been clearly identified. The reactivity of the ceria surface to CO₂ has been reported to be tuned by introducing CaO, which increases the number of basic sites for the ceria-based catalysts. However, the mechanism by which Ca²⁺ ions affect CO₂ decomposition is still debated. In this study, the morphologies and electronic properties of stoichiometric CeO₂(111), partially reduced CeO_2-x(111) (0 < x < 0.5), and calcium-doped ceria model catalysts, as well as their interactions with CO₂, were investigated by scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy, and synchrotron radiation photoemission spectroscopy. Stoichiometric CeO₂(111) and partially reduced CeO_2-x(111) films were epitaxially grown on a Cu(111) surface. STM images show that the stoichiometric CeO₂ film exhibits large, flat terraces that completely cover the Cu(111) surface. The reduced CeO_2-x film also has a flat surface and an ordered structure, but dark spaces are observed on the film. Different Ca-doped ceria films were prepared by physical vapor deposition of metallic Ca on CeO₂(111) at room temperature and subsequent annealing to 600 or 800 K in ultrahigh vacuum. The different preparation procedures produce samples with various surface components, oxidation states, and structures. Our results indicate that the deposition of metallic Ca on CeO₂ at room temperature leads to a partial reduction of Ce from the +4 to the +3 state, accompanied by the oxidation of Ca to Ca²⁺. Large CaO nanofilms are observed on CeO₂ upon annealing to 600 K. However, small CaO nanoislands appear near the step edges and more Ca²⁺ ions migrate into the subsurface of CeO₂ upon annealing to 800 K. In addition, different surface-adsorbed species are identified after CO₂ adsorption on ceria (CeO₂ and reduced CeO_2-x) and Ca-doped ceria films. CO₂ adsorption on the stoichiometric CeO₂ and partially reduced CeO_2-x surfaces leads to the formation of surface carboxylate. Moreover, the surface carboxylate species is more easily formed on reduced CeO_2-x with enhanced thermal stability than on stoichiometric CeO₂. On Ca-doped ceria films, the presence of Ca²⁺ ions is observed to be beneficial for CO₂ adsorption; further, the carbonate species is identified.
- Calcium,
- Ceria,
- Scanning tunneling microscopy,
- X-ray photoelectron spectroscopy,
- Synchrotron radiation photoemission spectroscopy
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Morphologies and Electronic Structures of Calcium-Doped Ceria Model Catalysts and Their Interaction with CO2

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Morphologies and Electronic Structures of Calcium-Doped Ceria Model Catalysts and Their Interaction with CO₂