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Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation

[Image: see text] Doping CeO(2) with Pd atoms has been associated with catalytic CO oxidation, but current surface models do not allow CO adsorption. Here, we report a new structure of Pd-doped CeO(2)(111), in which Pd adopts a square planar configuration instead of the previously assumed octahedral...

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Autores principales: Su, Ya-Qiong, Filot, Ivo A. W., Liu, Jin-Xun, Hensen, Emiel J. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5762167/
https://www.ncbi.nlm.nih.gov/pubmed/29333329
http://dx.doi.org/10.1021/acscatal.7b03295
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author Su, Ya-Qiong
Filot, Ivo A. W.
Liu, Jin-Xun
Hensen, Emiel J. M.
author_facet Su, Ya-Qiong
Filot, Ivo A. W.
Liu, Jin-Xun
Hensen, Emiel J. M.
author_sort Su, Ya-Qiong
collection PubMed
description [Image: see text] Doping CeO(2) with Pd atoms has been associated with catalytic CO oxidation, but current surface models do not allow CO adsorption. Here, we report a new structure of Pd-doped CeO(2)(111), in which Pd adopts a square planar configuration instead of the previously assumed octahedral configuration. Oxygen removal from this doped structure is favorable. The resulting defective Pd-doped CeO(2) surface is active for CO oxidation and is also able to cleave the first C–H bond in methane. We show how the moderate CO adsorption energy and dynamic features of the Pd atom upon CO adsorption and CO oxidation contribute to a low-barrier catalytic cycle for CO oxidation. These structures, which are also observed for Ni and Pt, can lead to a more open coordination environment around the doped-transition-metal center. These thermally stable structures are relevant to the development of single-atom catalysts.
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spelling pubmed-57621672018-01-11 Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation Su, Ya-Qiong Filot, Ivo A. W. Liu, Jin-Xun Hensen, Emiel J. M. ACS Catal [Image: see text] Doping CeO(2) with Pd atoms has been associated with catalytic CO oxidation, but current surface models do not allow CO adsorption. Here, we report a new structure of Pd-doped CeO(2)(111), in which Pd adopts a square planar configuration instead of the previously assumed octahedral configuration. Oxygen removal from this doped structure is favorable. The resulting defective Pd-doped CeO(2) surface is active for CO oxidation and is also able to cleave the first C–H bond in methane. We show how the moderate CO adsorption energy and dynamic features of the Pd atom upon CO adsorption and CO oxidation contribute to a low-barrier catalytic cycle for CO oxidation. These structures, which are also observed for Ni and Pt, can lead to a more open coordination environment around the doped-transition-metal center. These thermally stable structures are relevant to the development of single-atom catalysts. American Chemical Society 2017-11-20 2018-01-05 /pmc/articles/PMC5762167/ /pubmed/29333329 http://dx.doi.org/10.1021/acscatal.7b03295 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Su, Ya-Qiong
Filot, Ivo A. W.
Liu, Jin-Xun
Hensen, Emiel J. M.
Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title_full Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title_fullStr Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title_full_unstemmed Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title_short Stable Pd-Doped Ceria Structures for CH(4) Activation and CO Oxidation
title_sort stable pd-doped ceria structures for ch(4) activation and co oxidation
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5762167/
https://www.ncbi.nlm.nih.gov/pubmed/29333329
http://dx.doi.org/10.1021/acscatal.7b03295
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