Understanding selective hydrogenation of phenylacetylene on PdAg single atom alloy : DFT insights on molecule size and surface ensemble effects
Ibrahim, H. H., Weckman, T., Murzin, D. Y., & Honkala, K. (2024). Understanding selective hydrogenation of phenylacetylene on PdAg single atom alloy : DFT insights on molecule size and surface ensemble effects. Journal of Catalysis, 434, Article 115523. https://doi.org/10.1016/j.jcat.2024.115523
Julkaistu sarjassa
Journal of CatalysisPäivämäärä
2024Tekijänoikeudet
© 2024 the Authors
Single atom alloys (SAAs) have proven to be effective catalysts, offering customizable properties for diverse chemical processes. Various metal combinations are used in SAAs and Pd dispersed materials are frequently employed in catalyzing hydrogenation reactions. Herein, we explore the hydrogenation of phenylacetylene to styrene and ethylbenzene on PdAg SAA using density functional theory calculations. Our results show that while PdAg SAA does improve the activity of the host Ag towards hydrogenation, a dilute PdAg SAA surface with isolated Pd-atoms is not selective towards partial hydrogenation of phenylacetylene. Additionally, we investigate how the size of the reactant molecule, the size of the metal alloy ensemble, and the ligand effect impact the hydrogenation process. The SAA enhances the binding strengths of various organic adsorbates, although this effect diminishes as the adsorbate size increases. Our findings indicate the dilute PdAg exhibits selectivity towards hydrogenation of smaller molecules such acetylene due to its distinct adsorption geometry. The selective hydrogenation of phenylacetylene necessitates a surface Pd dimer ensemble. Our research highlights the importance of both reactant molecule size and surface configurations in SAA catalysts. This is particularly crucial when dealing with the adsorption of sizable organic molecules where the functional group can adopt different adsorption modes.
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Julkaisija
ElsevierISSN Hae Julkaisufoorumista
0021-9517Asiasanat
Julkaisuun liittyvä(t) tutkimusaineisto(t)
https://doi.org/10.23729/4fb60b0f-fe7b-4337-b5b0-af3a13f11b6dJulkaisu tutkimustietojärjestelmässä
https://converis.jyu.fi/converis/portal/detail/Publication/213695777
Metadata
Näytä kaikki kuvailutiedotKokoelmat
Rahoittaja(t)
Suomen Akatemia; Jane ja Aatos Erkon säätiöRahoitusohjelmat(t)
Elinkeinoelämän kanssa verkottunut tutkimus, BF; Akatemiaohjelma, SA; SäätiöLisätietoja rahoituksesta
The electronic structure calculations were made possible by computational resources provided by the CSC – IT Center for Science, Espoo, Finland (https://www.csc.fi/en/). HI and KH acknowledges Business Finland project Synjet and Finnish Research council, Finland project number 21000047181 for funding this work. TW and KH acknowledges Jane and Aatos Erkko Foundation, Finland for the funding for the LACOR project. ...Lisenssi
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