CO oxidation catalysed by Pd-based bimetallic nanoalloys
Density functional theory based global geometry optimization has been used to demonstrate the crucial influence of the geometry of the catalytic cluster on the energy barriers for the CO oxidation reaction over Pd-based bimetallic nanoalloys. We show that dramatic geometry change between the reactio...
| Main Authors: | , |
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| Format: | Journal article |
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Royal Society of Chemistry
2015
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| _version_ | 1797092704749879296 |
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| author | Palagin, D Doye, J |
| author_facet | Palagin, D Doye, J |
| author_sort | Palagin, D |
| collection | OXFORD |
| description | Density functional theory based global geometry optimization has been used to demonstrate the crucial influence of the geometry of the catalytic cluster on the energy barriers for the CO oxidation reaction over Pd-based bimetallic nanoalloys. We show that dramatic geometry change between the reaction intermediates can lead to very high energy barriers and thus be prohibitive for the whole process. This introduces challenges for both the design of new catalysts, and theoretical methods employed. On the theory side, a careful choice of geometric configurations of all reaction intermediates is crucial for an adequate description of a possible reaction path. From the point of view of the catalyst design, the cluster geometry can be controlled by adjusting the level of interaction between the cluster and the dopant metal, as well as between the adsorbate molecules and the catalyst cluster by mixing different metals in a single nanoalloy particle. We show that substitution of a Pd atom in the Pd$_{5}$ cluster with a single Ag atom to form Pd$_{4}$Ag$_{1}$ leads to a potential improvement of the catalytic properties of the cluster for the CO oxidation reaction. On the other hand, a single Au atom does not enhance the properties of the catalyst, which is attributed to a weaker hybridization between the cluster's constituent metals and the adsorbate molecules. Such flexibility of properties of bimetallic nanoalloy clusters illustrates the possibility of fine-tuning, which might be used for design of novel efficient catalytic materials. |
| first_indexed | 2024-03-07T03:49:48Z |
| format | Journal article |
| id | oxford-uuid:c0d6e30c-bb85-43fe-b709-7b97469e4189 |
| institution | University of Oxford |
| last_indexed | 2024-03-07T03:49:48Z |
| publishDate | 2015 |
| publisher | Royal Society of Chemistry |
| record_format | dspace |
| spelling | oxford-uuid:c0d6e30c-bb85-43fe-b709-7b97469e41892022-03-27T05:57:11ZCO oxidation catalysed by Pd-based bimetallic nanoalloysJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:c0d6e30c-bb85-43fe-b709-7b97469e4189Symplectic Elements at OxfordRoyal Society of Chemistry2015Palagin, DDoye, JDensity functional theory based global geometry optimization has been used to demonstrate the crucial influence of the geometry of the catalytic cluster on the energy barriers for the CO oxidation reaction over Pd-based bimetallic nanoalloys. We show that dramatic geometry change between the reaction intermediates can lead to very high energy barriers and thus be prohibitive for the whole process. This introduces challenges for both the design of new catalysts, and theoretical methods employed. On the theory side, a careful choice of geometric configurations of all reaction intermediates is crucial for an adequate description of a possible reaction path. From the point of view of the catalyst design, the cluster geometry can be controlled by adjusting the level of interaction between the cluster and the dopant metal, as well as between the adsorbate molecules and the catalyst cluster by mixing different metals in a single nanoalloy particle. We show that substitution of a Pd atom in the Pd$_{5}$ cluster with a single Ag atom to form Pd$_{4}$Ag$_{1}$ leads to a potential improvement of the catalytic properties of the cluster for the CO oxidation reaction. On the other hand, a single Au atom does not enhance the properties of the catalyst, which is attributed to a weaker hybridization between the cluster's constituent metals and the adsorbate molecules. Such flexibility of properties of bimetallic nanoalloy clusters illustrates the possibility of fine-tuning, which might be used for design of novel efficient catalytic materials. |
| spellingShingle | Palagin, D Doye, J CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title | CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title_full | CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title_fullStr | CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title_full_unstemmed | CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title_short | CO oxidation catalysed by Pd-based bimetallic nanoalloys |
| title_sort | co oxidation catalysed by pd based bimetallic nanoalloys |
| work_keys_str_mv | AT palagind cooxidationcatalysedbypdbasedbimetallicnanoalloys AT doyej cooxidationcatalysedbypdbasedbimetallicnanoalloys |