Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation
The active phase responsible for low-temperature CO oxidation in nanoparticulate CuO/CeO[subscript 2] catalysts was identified as surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x]. Contrary to previous studies, our measurements on a library of well-defined CuO/CeO[subscript 2] cat...
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| Format: | Article |
| Language: | en_US |
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American Chemical Society (ACS)
2017
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| Online Access: | http://hdl.handle.net/1721.1/109533 https://orcid.org/0000-0002-4347-0139 |
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| author | Bugnet, Matthieu Botton, Gianluigi A. Elias, Joseph Spanjaard Artrith, Nongnuch Giordano, Livia Kolpak, Alexie M. Shao-Horn, Yang |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Bugnet, Matthieu Botton, Gianluigi A. Elias, Joseph Spanjaard Artrith, Nongnuch Giordano, Livia Kolpak, Alexie M. Shao-Horn, Yang |
| author_sort | Bugnet, Matthieu |
| collection | MIT |
| description | The active phase responsible for low-temperature CO oxidation in nanoparticulate CuO/CeO[subscript 2] catalysts was identified as surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x]. Contrary to previous studies, our measurements on a library of well-defined CuO/CeO[subscript 2] catalysts have proven that the CuO phase is a spectator species, whereas the surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] phase is active for CO oxidation. Using in situ X-ray absorption spectroscopy, we found that the copper ions in Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] remain at high oxidation states (Cu[superscript 3+] and Cu[superscript 2+]) under oxygen-rich catalytic conditions without any evidence for Cu+. Artificial neural network potential Monte Carlo simulations suggest that Cu[superscript 3+] and Cu[superscript 2+] preferentially segregate to the {100} surface of the Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] nanoparticle, which is supported by aberration-corrected electron microscopy measurements. These results pave the way for understanding, at the atomic level, the mechanisms and descriptors pertinent for CO oxidation on these materials and hence the rational design of next-generation catalysts. |
| first_indexed | 2024-09-23T08:35:32Z |
| format | Article |
| id | mit-1721.1/109533 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T08:35:32Z |
| publishDate | 2017 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1095332022-09-30T09:50:14Z Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation Bugnet, Matthieu Botton, Gianluigi A. Elias, Joseph Spanjaard Artrith, Nongnuch Giordano, Livia Kolpak, Alexie M. Shao-Horn, Yang Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Department of Mechanical Engineering Massachusetts Institute of Technology. Research Laboratory of Electronics Shao-Horn, Yang Elias, Joseph Spanjaard Artrith, Nongnuch Giordano, Livia Kolpak, Alexie M. Shao-Horn, Yang The active phase responsible for low-temperature CO oxidation in nanoparticulate CuO/CeO[subscript 2] catalysts was identified as surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x]. Contrary to previous studies, our measurements on a library of well-defined CuO/CeO[subscript 2] catalysts have proven that the CuO phase is a spectator species, whereas the surface-substituted Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] phase is active for CO oxidation. Using in situ X-ray absorption spectroscopy, we found that the copper ions in Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] remain at high oxidation states (Cu[superscript 3+] and Cu[superscript 2+]) under oxygen-rich catalytic conditions without any evidence for Cu+. Artificial neural network potential Monte Carlo simulations suggest that Cu[superscript 3+] and Cu[superscript 2+] preferentially segregate to the {100} surface of the Cu[subscript y]Ce[subscript 1–y]O[subscript 2–x] nanoparticle, which is supported by aberration-corrected electron microscopy measurements. These results pave the way for understanding, at the atomic level, the mechanisms and descriptors pertinent for CO oxidation on these materials and hence the rational design of next-generation catalysts. National Science Foundation (U.S.) (grant number ACI-1053575) United States. Department of Energy. Office of Science (Contract No. DE-AC02- 05CH11231) United States. Department of Energy. Office of Basic Energy Sciences (Contract No. DE-AC02-98CH10886) Philip Morris International National Science Foundation (U.S.) (Graduate Research Fellowship under Grant No. DGE-1122374) Schlumberger Foundation. Faculty for the Future (fellowship) 2017-06-02T14:31:45Z 2017-06-02T14:31:45Z 2016-02 Article http://purl.org/eprint/type/JournalArticle 2155-5435 2155-5435 http://hdl.handle.net/1721.1/109533 Elias, Joseph S., Nongnuch Artrith, Matthieu Bugnet, Livia Giordano, Gianluigi A. Botton, Alexie M. Kolpak, and Yang Shao-Horn. “Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation.” ACS Catalysis 6, no. 3 (March 4, 2016): 1675–1679. https://orcid.org/0000-0002-4347-0139 en_US http://dx.doi.org/10.1021/acscatal.5b02666 ACS Catalysis Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) Prof. Shao-Horn via Angie Locknar |
| spellingShingle | Bugnet, Matthieu Botton, Gianluigi A. Elias, Joseph Spanjaard Artrith, Nongnuch Giordano, Livia Kolpak, Alexie M. Shao-Horn, Yang Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title | Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title_full | Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title_fullStr | Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title_full_unstemmed | Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title_short | Elucidating the Nature of the Active Phase in Copper/Ceria Catalysts for CO Oxidation |
| title_sort | elucidating the nature of the active phase in copper ceria catalysts for co oxidation |
| url | http://hdl.handle.net/1721.1/109533 https://orcid.org/0000-0002-4347-0139 |
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