Detailed Process of Adsorption of Alkanes and Alkenes on Zeolites

Yoda, Eisuke; Kondo, Junko N.; Domen, Kazunari

doi:10.1021/jp047376+

Cited by 61 publications

(72 citation statements)

References 34 publications

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“…[ [36][37][38] The elastic incoherent scattering function (EISF) allows the intensity of the individual quasi-elastic components to be compared with the elastic component (Figure 8). The EISF for the component corresponding to jump diffusion of free ethanol (Figure 8a), decreases at higher temperatures, showing an increase in the relative intensity of this component with respect to the elastic component.…”

Section: Quasi-elastic Neutron Scattering Of Ethanol and Ethermentioning

confidence: 99%

Spectroscopic investigation into the design of solid–acid catalysts for the low temperature dehydration of ethanol

Potter

Aswegen

Gibson

et al. 2016

Phys. Chem. Chem. Phys.

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The increased demand for bulk hydrocarbons necessitates research into increasingly sustainable, energy-efficient catalytic processes. Owing to intricately designed structure-property correlations, SAPO-34 has become established as a promising material for the low temperature ethanol dehydration to produce ethylene. However, further optimization of this process requires a precise knowledge of the reaction mechanism at a molecular level. In order to achieve this a range of spectroscopic characterization techniques are required to probe both the interaction with the active site, and also the wider role of the framework. To this end we employ a combination of in situ infra-red and neutron scattering techniques to elucidate the influence of the surface ethoxy species in the activation of both diethyl ether and ethanol, towards the improved formation of ethylene at low temperatures. The combined conclusions of these studies is that the formation of ethylene is the rate determining step, which is of fundamental importance towards the development of this process and the introduction of bio-ethanol as a viable feedstock for ethylene production.

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Section: Quasi-elastic Neutron Scattering Of Ethanol and Ethermentioning

confidence: 99%

Spectroscopic investigation into the design of solid–acid catalysts for the low temperature dehydration of ethanol

Potter

Aswegen

Gibson

et al. 2016

Phys. Chem. Chem. Phys.

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“…For butenes some NMR and infrared based adsorption studies are available. The adsorption of butenes on H-ZSM-5 and mordenite was experimentally investigated by Domen et al [12,13,[17][18][19]. On H-ZSM-5, they observed that at sub-ambient temperatures a stable p-complex was formed and that double bond isomerization occurred already at 230 K [13,18,20].…”

Section: Introductionmentioning

confidence: 99%

On the stability and nature of adsorbed pentene in Brønsted acid zeolite H-ZSM-5 at 323 K

Hajek

Mynsbrugge

Wispelaere

et al. 2016

Journal of Catalysis

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Herewith we have the pleasure to resubmit the paper entitled : "On the stability and nature of adsorbed pentene in Brønsted acid zeolite H-ZSM-5 at 323 K" by J. Hajek , J. Van der Mynsbrugge, K. De Wispelaere , P. Cnudde, L. Vanduyfhuys, M. Waroquier and V. Van Speybroeck, for publication in Journal of Catalysis.We have received the comments of two reviewers which were very positive and which suggest publication subject to some major/minor revisions. We have taken them all into account in the revised version. In separate documents we give a substantial reply to the reviewers that carefully addresses the issues raised in the reviewer's comments. We have added an author (Louis Vanduyfhuys) in the list. During the revision process he has given a very constructive contribution in a correct thermodynamic analysis of the metadynamics results. As requested by one of the reviewers, we re-analyzed all our MD results. We hope that you are willing to accept this slight change in the author list.We further hope that the manuscript is now suitable for publication. Reply to reviewer #1 :We thank the reviewer for his/her careful reading of the manuscript with manuscript number JCAT-16-151. We try to give a valuable reply to all comments which were all very constructive. Reviewer's comments are printed in blue.1. The DFT calculations have been carried out at 0 K by optimizing the geometry at the RPBE+D3 level and then conducting single point calculations with other functionals. While the general conclusions drawn from the calculations are independent of the functional chosen, it would be very useful to know whether geometry optimization with a better functional would change the conclusion about the relative stability of the -complex and alkoxide structures.The authors completely agree with the major concern of the reviewer regarding the reliability of the geometry optimization based on one level of theory (PBE+D3). This functional has proven to be reliable in many periodic static calculations on nanoporous materials, but to remove any doubt we performed new geometry optimizations and frequency calculations for 2-pentene π-complex and 2-pentoxide using BEEF-vdW functional .[1] Geometrical details of the selected structures with PBE-D3 and BEEF-vdW functionals are given in Table 1. The comparison of free energy ΔG and enthalpy ΔH differences between BEEF-vdW //PBE D3 and BEEF-vdW // BEEF-vdW is given in Table 2. The energy differences are very similar with each other, and support the conclusions made in the paper. These additional results have been included in *Revision NotesWe thank the reviewer for this remark and reformulated the sentence slightly. The origin of larger adsorption enthalpies for the -complex is indeed related to usage of optimized geometries, which take into account only one point on the potential energy surface. Our MD simulations show that in reality at finite temperatures, the -complex can adopt various geometries leading to a probability distribution as shown in Figure 3 of the main manuscript. This dis...

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“…Recently, experimental investigations in molecular details of structures and adsorption dynamics and interaction energies of hydrocarbons in zeolites have been reported [12][13][14][15][16][17][18]. It was found that the pore size of zeolites had strong effects on the geometries of adsorption sites, the structures of the adsorption complexes, and the adsorption energies.…”

Section: Introductionmentioning

confidence: 99%

“…The linear correlations of interaction energy (heat of adsorption) and the number of carbon atoms of n-alkanes have been found in various zeolites [19]. However, the adsorption of alkenes in acidic zeolites is complicated by the rapid reactions of oligomerization and isomerization at the Brønsted acid sites [17,18,20]. The heat of adsorption of alkenes cannot be experimentally measured because of these reactions.…”

Section: Introductionmentioning

confidence: 99%

The adsorption of saturated and unsaturated hydrocarbons on nanostructured zeolites (H-MOR and H-FAU): An ONIOM study

Pantu¹,

Boekfa²,

Limtrakul³

2007

Journal of Molecular Catalysis A: Chemical

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Detailed Process of Adsorption of Alkanes and Alkenes on Zeolites

Cited by 61 publications

References 34 publications

Spectroscopic investigation into the design of solid–acid catalysts for the low temperature dehydration of ethanol

Spectroscopic investigation into the design of solid–acid catalysts for the low temperature dehydration of ethanol

On the stability and nature of adsorbed pentene in Brønsted acid zeolite H-ZSM-5 at 323 K

The adsorption of saturated and unsaturated hydrocarbons on nanostructured zeolites (H-MOR and H-FAU): An ONIOM study

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