Theoretical and experimental investigations into light alkane dehydrogenation over chromium-containing catalyst

Du, Yiqing; Wang, Yanxiao; Zhang, Chengtao; Li, Rongzhao; Wang, Bo; Li, Shuo; Yang, Chaohe

doi:10.1016/j.fuel.2022.123893

Cited by 7 publications

(2 citation statements)

References 62 publications

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“…Factor 2 in the equation accounts for the two identical surfaces, i. e., top and bottom. Surface energies for Pt(111) and Ru(0001) converged at 2.40 and 3.33 J/m 2 , respectively, which are in good agreement with the previous calculated [30,40,41] and experimental values [40,42] (Table S1 in the Supporting Information). Accordingly, Pt(111) was modeled with a 4-layer slab with 4×4 supercell size where the bottom two layers were frozen at the optimized bulk lattice.…”

Section: Models and Computational Methodssupporting

confidence: 88%

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Islam,

Catlow,

Roldan

2024

ChemCatChem

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The dehydrogenation of alkanes is a critical process to enable olefin upcycling in a circular economy. A suitable selective catalyst is required in order to avoid demanding reaction conditions and ensure the activation of the C–H bond rather than breaking the C–C bond, which is the weaker of the two. Herein, using periodic density functional theory, we have investigated the dehydrogenation of n‐pentane (as a model compound) on Pt and Ru surface catalysts. The results show that the first dehydrogenation occurs through the dissociative adsorption of the C–H bond, resulting in pentyl and H intermediates on the metal surfaces. A successive dehydrogenation creates pentene via a hydride di‐σ state, leaving the abstracted hydrogen atoms on the metal surfaces. In agreement with recent experiments, Pt and Ru catalysts show a similar reactivity trend: pentane dehydrogenation yields pent‐1‐ene and pent‐2‐ene. The simulations reveal that the 1st C–H dissociation is the rate‐determining step, whereas the double‐bonded alkenes (pent‐1‐ene and pent‐2‐ene) are formed due to fast successive dehydrogenation processes. Pt favors the formation of pent‐1‐ene, whereas Ru favors the formation of pent‐2‐ene.

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Section: Models and Computational Methodssupporting

confidence: 88%

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Islam,

Catlow,

Roldan

2024

ChemCatChem

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“…Concerted Mechanism. It has been reported that after doping the γ-Al 2 O 3 surface with Ga species, the alkane dehydrogenation generally follows two different reaction mechanisms, i.e., the stepwise and concerted mechanisms, depending on the influence of surface geometric and electronic structures 33,57,58. Unlike the stepwise mechanism, the two C− H bonds from the central and terminal carbons in propane are cleaved simultaneously during the concerted mechanism, skipping the intermediate step of 2-propyl formation.…”

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confidence: 99%

Enhanced C–H Bond Activation by a Concerted Mechanism: A Comparative Microkinetic Analysis of Propane Dehydrogenation over Single-Pt-Doped θ- and γ-Al₂O₃ Catalysts

Hu,

Zeeshan,

Yang

et al. 2024

Ind. Eng. Chem. Res.

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Alumina is among the most widely used supports in the field of heterogeneous catalysis. In this work, DFT calculations and microkinetic analysis have been combined to examine the catalytic behaviors of θ- and γ-Al2O3-supported Pt single atom catalysts in propane dehydrogenation (PDH). Calculated results indicate oxygen vacancies may weaken the Lewis acid–base interactions between a pair of coadsorbed amphoteric species at the Al–O sites. Although the coadsorption cannot be strengthened at the Pt–O sites, the reaction intermediates involved are bound most tightly at the Pt sites. A concerted mechanism in which two C–H bonds are simultaneously activated is proposed on Pt-doped θ-Al2O3, which dominates the stepwise mechanism and gives rise to a high activity. In contrast, PDH cannot take place along the concerned pathway on Pt-doped γ-Al2O3 because of the large surface distortion induced. These results provide a rational interpretation of the superior PDH performance of the θ-Al2O3-supported Pt catalyst.

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Core-shell equivalent reactor network model to bridging CFD and process simulations of a fluidized bed reactor

Du,

Cheng,

et al. 2024

Chemical Engineering Science

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Theoretical and experimental investigations into light alkane dehydrogenation over chromium-containing catalyst

Cited by 7 publications

References 62 publications

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Enhanced C–H Bond Activation by a Concerted Mechanism: A Comparative Microkinetic Analysis of Propane Dehydrogenation over Single-Pt-Doped θ- and γ-Al₂O₃ Catalysts

Core-shell equivalent reactor network model to bridging CFD and process simulations of a fluidized bed reactor

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Theoretical and experimental investigations into light alkane dehydrogenation over chromium-containing catalyst

Cited by 7 publications

References 62 publications

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Mechanistic Pathways for the Dehydrogenation of Alkanes on Pt(111) and Ru(0001) Surfaces

Enhanced C–H Bond Activation by a Concerted Mechanism: A Comparative Microkinetic Analysis of Propane Dehydrogenation over Single-Pt-Doped θ- and γ-Al2O3 Catalysts

Core-shell equivalent reactor network model to bridging CFD and process simulations of a fluidized bed reactor

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Enhanced C–H Bond Activation by a Concerted Mechanism: A Comparative Microkinetic Analysis of Propane Dehydrogenation over Single-Pt-Doped θ- and γ-Al₂O₃ Catalysts