A1 Journal article (refereed)
Understanding selective hydrogenation of phenylacetylene on PdAg single atom alloy : DFT insights on molecule size and surface ensemble effects (2024)

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

JYU authors or editors

Publication details

All authors or editors: Ibrahim, Hanan H.; Weckman, Timo; Murzin, Dmitry Yu.; Honkala, Karoliina

Journal or series: Journal of Catalysis

ISSN: 0021-9517

eISSN: 1090-2694

Publication year: 2024

Publication date: 30/04/2024

Volume: 434

Article number: 115523

Publisher: Elsevier

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1016/j.jcat.2024.115523

Research data link: https://doi.org/10.23729/4fb60b0f-fe7b-4337-b5b0-af3a13f11b6d

Publication open access: Openly available

Publication channel open access: Partially open access channel

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/95037

Web address of parallel published publication (pre-print): https://doi.org/10.26434/chemrxiv-2024-7mq3w

Abstract

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.

Keywords: density functional theory; chemical reactions; catalysis; catalysts

Free keywords: density functional theory; single atom alloy; PdAg; phenylacetylene

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Ministry reporting: Yes

Reporting Year: 2024

Preliminary JUFO rating: 3