Shape-dependent interplay between oxygen vacancies and Ag–CeO2 interaction in Ag/CeO2 catalysts and their influence on the catalytic activity
The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal the shape-dependent interplay between oxygen vacancies and Ag-CeO2 interaction and their influence on the catalytic activity. Silver supported...
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| Published in: | Journal of catalysis Vol. 293; pp. 195 - 204 |
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| Main Authors: | , , , , , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
Amsterdam
Elsevier Inc
01-09-2012
Elsevier Elsevier BV |
| Subjects: | |
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| Abstract | The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal the shape-dependent interplay between oxygen vacancies and Ag-CeO2 interaction and their influence on the catalytic activity. Silver supported on CeO2 nanocubes with a loading of 1% shows the highest specific catalytic activity. [Display omitted]
► The interplay between oxygen vacancies and Ag–CeO2 interaction depends on the shape of CeO2. ► Such an interplay controls the structures and catalytic activity of Ag/CeO2 catalysts. ► CeO2 nanorods stabilize cationic Ag species. ► CeO2 nanocubes facilitate the formation of metallic Ag nanoparticles. ► The Ag nanoparticle–CeO2 interface is the active structure in catalyzing CO oxidation.
Ag/CeO2 catalysts employing CeO2 nanocubes (c-CeO2) and nanorods (r-CeO2) as the support were prepared by conventional incipient wetness impregnation followed by calcination at 500°C in air. Their structures have been characterized in detail and their catalytic activities in CO oxidation have also been tested. c-CeO2 and r-CeO2 nanocrystals exhibit different concentrations and structures of oxygen vacancies. The silver-r-CeO2 interaction is stronger than the silver-c-CeO2 interaction. Fine Ag nanoparticles form in 1%-Ag/c-CeO2 and grow in size in 3%-Ag/c-CeO2; however, positively charged Agn+ clusters dominate in 1%-Ag/r-CeO2, and fine Ag nanoparticles dominate in 3%-Ag/r-CeO2. Supported Ag nanoparticles are much more capable of creating oxygen vacancies in CeO2 than supported positively charged Agn+ clusters. More oxygen vacancies form in Ag/c-CeO2 than in Ag/r-CeO2. The average charge density of oxygen vacancies and the ratio between large oxygen vacancy clusters and small vacancies in CeO2 nanocrystals are enhanced when loaded with positively charged Agn+ clusters but reduced when loaded with Ag nanoparticles. Ag nanoparticles greatly promote the reduction and catalytic activity in CO oxidation of CeO2 nanocrystals but positively charged Agn+ clusters do not. These results demonstrate the concept that the interplay between oxygen vacancies and Ag–CeO2 interaction controls the structures of silver and CeO2 in Ag/CeO2 catalysts and thus their surface reactivity and catalytic activity, deepening the fundamental understanding of metal/CeO2 catalysts. These results also reveal that the interplay between oxygen vacancies and Ag–CeO2 interaction in Ag/CeO2 catalysts depends on the shape of CeO2 support, opening up a new strategy for the design of efficient and economic metal/CeO2 catalysts by engineering the shape of CeO2 support. |
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| AbstractList | The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal the shape-dependent interplay between oxygen vacancies and Ag-CeO2 interaction and their influence on the catalytic activity. Silver supported on CeO2 nanocubes with a loading of 1% shows the highest specific catalytic activity. [Display omitted]
► The interplay between oxygen vacancies and Ag–CeO2 interaction depends on the shape of CeO2. ► Such an interplay controls the structures and catalytic activity of Ag/CeO2 catalysts. ► CeO2 nanorods stabilize cationic Ag species. ► CeO2 nanocubes facilitate the formation of metallic Ag nanoparticles. ► The Ag nanoparticle–CeO2 interface is the active structure in catalyzing CO oxidation.
Ag/CeO2 catalysts employing CeO2 nanocubes (c-CeO2) and nanorods (r-CeO2) as the support were prepared by conventional incipient wetness impregnation followed by calcination at 500°C in air. Their structures have been characterized in detail and their catalytic activities in CO oxidation have also been tested. c-CeO2 and r-CeO2 nanocrystals exhibit different concentrations and structures of oxygen vacancies. The silver-r-CeO2 interaction is stronger than the silver-c-CeO2 interaction. Fine Ag nanoparticles form in 1%-Ag/c-CeO2 and grow in size in 3%-Ag/c-CeO2; however, positively charged Agn+ clusters dominate in 1%-Ag/r-CeO2, and fine Ag nanoparticles dominate in 3%-Ag/r-CeO2. Supported Ag nanoparticles are much more capable of creating oxygen vacancies in CeO2 than supported positively charged Agn+ clusters. More oxygen vacancies form in Ag/c-CeO2 than in Ag/r-CeO2. The average charge density of oxygen vacancies and the ratio between large oxygen vacancy clusters and small vacancies in CeO2 nanocrystals are enhanced when loaded with positively charged Agn+ clusters but reduced when loaded with Ag nanoparticles. Ag nanoparticles greatly promote the reduction and catalytic activity in CO oxidation of CeO2 nanocrystals but positively charged Agn+ clusters do not. These results demonstrate the concept that the interplay between oxygen vacancies and Ag–CeO2 interaction controls the structures of silver and CeO2 in Ag/CeO2 catalysts and thus their surface reactivity and catalytic activity, deepening the fundamental understanding of metal/CeO2 catalysts. These results also reveal that the interplay between oxygen vacancies and Ag–CeO2 interaction in Ag/CeO2 catalysts depends on the shape of CeO2 support, opening up a new strategy for the design of efficient and economic metal/CeO2 catalysts by engineering the shape of CeO2 support. Ag/CeO₂ catalysts employing CeO₂ nanocubes (c-CeO₂) and nanorods (r-CeO₂) as the support were prepared by conventional incipient wetness impregnation followed by calcination at 500°C in air. Their structures have been characterized in detail and their catalytic activities in CO oxidation have also been tested. c-CeO₂ and r-CeO₂ nanocrystals exhibit different concentrations and structures of oxygen vacancies. The silver-r-CeO₂ interaction is stronger than the silver-c-CeO₂ interaction. Fine Ag nanoparticles form in 1%-Ag/c-CeO₂ and grow in size in 3%-Ag/c-CeO₂; however, positively charged Agₙ ⁺ clusters dominate in 1%-Ag/r-CeO₂, and fine Ag nanoparticles dominate in 3%-Ag/r-CeO₂. Supported Ag nanoparticles are much more capable of creating oxygen vacancies in CeO₂ than supported positively charged Agₙ ⁺ clusters. More oxygen vacancies form in Ag/c-CeO₂ than in Ag/r-CeO₂. The average charge density of oxygen vacancies and the ratio between large oxygen vacancy clusters and small vacancies in CeO₂ nanocrystals are enhanced when loaded with positively charged Agₙ ⁺ clusters but reduced when loaded with Ag nanoparticles. Ag nanoparticles greatly promote the reduction and catalytic activity in CO oxidation of CeO₂ nanocrystals but positively charged Agₙ ⁺ clusters do not. These results demonstrate the concept that the interplay between oxygen vacancies and Ag–CeO₂ interaction controls the structures of silver and CeO₂ in Ag/CeO₂ catalysts and thus their surface reactivity and catalytic activity, deepening the fundamental understanding of metal/CeO₂ catalysts. These results also reveal that the interplay between oxygen vacancies and Ag–CeO₂ interaction in Ag/CeO₂ catalysts depends on the shape of CeO₂ support, opening up a new strategy for the design of efficient and economic metal/CeO₂ catalysts by engineering the shape of CeO₂ support. Graphical abstract The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal the shape-dependent interplay between oxygen vacancies and Ag-CeO2 interaction and their influence on the catalytic activity. Silver supported on CeO2 nanocubes with a loading of 1% shows the highest specific catalytic activity. Display Omitted Highlights The interplay between oxygen vacancies and Ag-CeO2 interaction depends on the shape of CeO2 . Such an interplay controls the structures and catalytic activity of Ag/CeO2 catalysts. CeO2 nanorods stabilize cationic Ag species. CeO2 nanocubes facilitate the formation of metallic Ag nanoparticles. The Ag nanoparticle-CeO2 interface is the active structure in catalyzing CO oxidation. [PUBLICATION ABSTRACT] |
| Author | Ma, Yunsheng Ye, Bangjiao Huang, Weixin Chang, Sujie Hua, Qing Zhang, Lijuan Li, Mo |
| Author_xml | – sequence: 1 givenname: Sujie surname: Chang fullname: Chang, Sujie organization: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China – sequence: 2 givenname: Mo surname: Li fullname: Li, Mo organization: Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China – sequence: 3 givenname: Qing surname: Hua fullname: Hua, Qing organization: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China – sequence: 4 givenname: Lijuan surname: Zhang fullname: Zhang, Lijuan organization: Department of Modern Physics, University of Science and Technology of China, Hefei 230026, China – sequence: 5 givenname: Yunsheng surname: Ma fullname: Ma, Yunsheng organization: Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China – sequence: 6 givenname: Bangjiao surname: Ye fullname: Ye, Bangjiao organization: Department of Modern Physics, University of Science and Technology of China, Hefei 230026, China – sequence: 7 givenname: Weixin surname: Huang fullname: Huang, Weixin email: huangwx@ustc.edu.cn organization: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China |
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| Keywords | Metal–support interaction Active structure Shape dependence CO oxidation Ag/CeO2 catalysts Oxygen vacancy Metal support interaction Binary compound Shape Support Nanoparticle Cerium oxide Lanthanide compound Design Chemical reduction catalysts Oxidation Metal-support interaction Chemical reactivity Structure Nanorod Nanocrystal Oxygen Catalytic reaction Vacancy Ag/CeO Transition metal Air Charge density Silver Heterogeneous catalysis Impregnation Catalyst |
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| Snippet | The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal... Ag/CeO₂ catalysts employing CeO₂ nanocubes (c-CeO₂) and nanorods (r-CeO₂) as the support were prepared by conventional incipient wetness impregnation followed... Graphical abstract The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The... |
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| SubjectTerms | Active structure Ag/CeO2 catalysts air carbon monoxide Catalysis Catalysts catalytic activity ceric oxide Chemistry CO oxidation Colloidal state and disperse state engineering Exact sciences and technology General and physical chemistry Metal–support interaction nanocrystals nanorods nanosilver oxidation Oxygen Oxygen vacancy Physical and chemical studies. Granulometry. Electrokinetic phenomena Shape dependence silver Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
| Title | Shape-dependent interplay between oxygen vacancies and Ag–CeO2 interaction in Ag/CeO2 catalysts and their influence on the catalytic activity |
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