Effect of Oxidized Tin Interfacial Atoms on Methylcyclohexane Dehydrogenation Catalyzed by γ‐Alumina Supported Platinum Clusters - Archive ouverte HAL
Journal Articles ChemCatChem Year : 2024

Effect of Oxidized Tin Interfacial Atoms on Methylcyclohexane Dehydrogenation Catalyzed by γ‐Alumina Supported Platinum Clusters

Masoud Shahrokhi
Céline Chizallet
David Loffreda

Abstract

Abstract Tin (Sn) doped platinum (Pt) nanoparticles supported on γ‐alumina are important materials catalyzing various reactions, such as the dehydrogenation of methylcyclohexane (MCH) into toluene, involved in liquid organic hydrogen carriers process, and naphtha catalytic reforming. The role of oxidized forms of Sn, remains misunderstood. Relying on catalysts' models made of a Pt 13 cluster on the (100) surface of γ‐alumina, the location and effects of Sn 4+ and Sn 2+ interfacial atoms are investigated by density functional theory (DFT) calculations. A simulated annealing approach based on ab initio molecular dynamics enables to explore the configurations of the catalytic systems. The Pt clusters' stabilities and that of the adsorbed molecular intermediates are linked to the electronic properties of the cluster and to its ductility modulated by the adsorbed species, the alumina support and the Sn atoms. The Gibbs free energy profiles related to the reaction mechanism of the MCH dehydrogenation into toluene are quantified on the basis of transition state search. The energy span concept reveals that the dual (either detrimental or beneficial) impact of Sn oxidized forms on the intrinsic reactivity of the Pt 13 cluster depends on temperature. Based on this DFT analysis, we attempt to clarify the debated role of Sn oxidized species.
Embargoed file
Embargoed file
0 4 6
Year Month Jours
Avant la publication
Thursday, March 20, 2025
Embargoed file
Thursday, March 20, 2025
Please log in to request access to the document

Dates and versions

hal-04747228 , version 1 (21-10-2024)

Identifiers

Cite

Masoud Shahrokhi, Céline Chizallet, David Loffreda, Pascal Raybaud. Effect of Oxidized Tin Interfacial Atoms on Methylcyclohexane Dehydrogenation Catalyzed by γ‐Alumina Supported Platinum Clusters. ChemCatChem, 2024, pp.e202401300. ⟨10.1002/cctc.202401300⟩. ⟨hal-04747228⟩
0 View
0 Download

Altmetric

Share

More