Dehydration of butanol towards butenes over MFI, FAU and MOR: influence of zeolite topology

Reviere, Arno de; Gunst, Dieter; Sabbe, Maarten; Reyniers, Marie-Françoise; Verberckmoes, An

doi:10.1039/d0cy02366c

Cited by 20 publications

(19 citation statements)

References 64 publications

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“…Furthermore, Buniazet et al [13] ruled out ether-mediated mechanisms (in-termolecular dehydration) to explain the formation of linear butenes, which was based on the fact that the thermal evolution of the selectivity to linear butenes measured experimentally was not found to follow the evolution of the rate of ether formation predicted by density functional theory (DFT) calculations [25]. This absence of ether-mediated mechanism is also corroborated in the case of isobutanol dehydration in ZSM-5, faujasite and mordenite [26,27].…”

Section: Introductionmentioning

confidence: 96%

Monomolecular mechanisms of isobutanol conversion to butenes catalyzed by acidic zeolites: Alcohol isomerization as a key to the production of linear butenes

Gešvandtnerová

Raybaud

Chizallet

2022

Journal of Catalysis

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Section: Introductionmentioning

confidence: 96%

Monomolecular mechanisms of isobutanol conversion to butenes catalyzed by acidic zeolites: Alcohol isomerization as a key to the production of linear butenes

Gešvandtnerová

Raybaud

Chizallet

2022

Journal of Catalysis

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“…[ 23 ] Further in situ adsorption of isobutanol was carried out to identify the formation of short‐range crystalline order in the silicate structure containing 5MRs after short time of HT. [ 25 ] Figure 2b shows FTIR spectra of isobutanol adsorbed in the calcined samples, where the characteristic CH 3 and CH 2 stretching vibration bands between 3000 and 2800 cm −1 are evident. [ 26 ] For the Fe@Si sample, isobutanol is only adsorbed on silanol groups as indicated by the presence of a band at 3745 cm −1 .…”

Section: Resultsmentioning

confidence: 99%

Synthesis of Core–Shell Magnetic Nanoparticles Containing Ultrasmall Domains of Silicalite‐1

Piva

Ghojavand

et al. 2022

Adv Materials Inter

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Synthesis of core-shell nanostructures with magnetic core and zeolitic shell is an ongoing challenge. Herein, we present a strategy for preparation of -Fe2O3@mesoporous silica (mSiO2) core-shell nanoparticles containing ultra-small domains of silicalite-1 in the shell (-Fe2O3@mSiO2/Silicalite-1). The strategy consists in a solid-state reorganization of the precursor amorphous mSiO2 shell into silicalite-1 using a tetrapropylammonium hydroxide (TPAOH) as an organic structure-directing agent (OSDA) under mild hydrothermal (HT) 2 conditions. The formation of sililicalite-1 crystalline domains has been investigated through the detailed characterization of products obtained at different times of HT treatment by XRD, Raman spectroscopy, FTIR, SEM with EDS, TEM and nitrogen physisorption. By careful tuning the time of HT treatment, the -Fe2O3@mSiO2/Silicalite-1 nanostructures are prepared.

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“…For example, the 8MR pocket of mordenite was found to be unsuitable for the formation of ethers, contrary to the 12MR channel. 674 The ether formation route is strongly inhibited in zeolites exhibiting 8MR pores (e.g., mordenite) for ethanol, 674,675 1-butanol, and isobutanol, 676 where only the corresponding alkene is formed. In zeolites with larger pores, such as ZSM-5 and faujasite, the intermolecular route is favored, and the ether is the major product in some cases, in particular with ethanol below 550 K. 611,674 Intermolecular dehydration is expected to take place by nucleophilic substitution.…”

Section: Bimolecular Mechanisms: Formation Of Ethers and Their Decomp...mentioning

confidence: 99%

Molecular Views on Mechanisms of Brønsted Acid-Catalyzed Reactions in Zeolites

et al. 2023

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The Brønsted acidity of proton-exchanged zeolites has historically led to the most impactful applications of these materials in heterogeneous catalysis, mainly in the fields of transformations of hydrocarbons and oxygenates. Unravelling the mechanisms at the atomic scale of these transformations has been the object of tremendous efforts in the last decades. Such investigations have extended our fundamental knowledge about the respective roles of acidity and confinement in the catalytic properties of proton exchanged zeolites. The emerging concepts are of general relevance at the crossroad of heterogeneous catalysis and molecular chemistry. In the present review, emphasis is given to molecular views on the mechanism of generic transformations catalyzed by Brønsted acid sites of zeolites, combining the information gained from advanced kinetic analysis, in situ, and operando spectroscopies, and quantum chemistry calculations. After reviewing the current knowledge on the nature of the Brønsted acid sites themselves, and the key parameters in catalysis by zeolites, a focus is made on reactions undergone by alkenes, alkanes, aromatic molecules, alcohols, and polyhydroxy molecules. Elementary events of C–C, C–H, and C–O bond breaking and formation are at the core of these reactions. Outlooks are given to take up the future challenges in the field, aiming at getting ever more accurate views on these mechanisms, and as the ultimate goal, to provide rational tools for the design of improved zeolite-based Brønsted acid catalysts.

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Dehydration of butanol towards butenes over MFI, FAU and MOR: influence of zeolite topology

Abstract: The effect zeolite topologies have on different types of reactions is one of the fundamental aspects that has made zeolite catalysts immensely popular at an industrial level. Yet, the influence...

Cited by 20 publications

References 64 publications

Monomolecular mechanisms of isobutanol conversion to butenes catalyzed by acidic zeolites: Alcohol isomerization as a key to the production of linear butenes

Monomolecular mechanisms of isobutanol conversion to butenes catalyzed by acidic zeolites: Alcohol isomerization as a key to the production of linear butenes

Synthesis of Core–Shell Magnetic Nanoparticles Containing Ultrasmall Domains of Silicalite‐1

Molecular Views on Mechanisms of Brønsted Acid-Catalyzed Reactions in Zeolites

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