Room temperature methoxylation in zeolites: insight into a key step of the methanol-to-hydrocarbons process

O’Malley, Alexander J.; Parker, Stewart F.; Chutia, Arunabhiram; Farrow, Matthew R.; Silverwood, Ian P.; García-Sakai, Victoria; Catlow, C. Richard A.

doi:10.1039/c5cc08956e

Cited by 61 publications

(88 citation statements)

References 46 publications

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“…Molecular dynamics (MD) simulations have also been used to model the diffusion of alkanes into MFI zeolites, as measured by means of QENS and neutron spin‐echo (NSE) . Methanol diffusion (QENS), reaction, and adsorption (INS) during the methanol‐to‐hydrocarbon process have also been studied …”

Section: Hydrogen Interactions With Oxide Catalystsmentioning

confidence: 99%

Neutron Scattering Investigations of Hydride Species in Heterogeneous Catalysis

et al. 2018

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In heterogeneous catalysis, hydrides on the surface or in the bulk play a critical role as either active components or reaction intermediates in many hydrogen‐involving reactions, but characterization of the nature and structure of these hydride species remains challenging. Neutron scattering, which is extremely sensitive to light elements, such as hydrogen, has shown great potential in meeting this challenge. In this Minireview, recent advances in neutron studies of hydride species, mainly over the two most typical classes of catalysts—metals and oxides—are surveyed. Findings on catalysts outside these categories are raised if they are considered to be relevant for contextualization in the present Minireview. The adsorption, dissociation, spillover, and reactivity of hydrogen, especially hydride species over supported metal and oxide catalysts, have been successfully investigated, mostly by means of neutron vibrational spectroscopy. Insights from these neutron studies, which are otherwise not possible with other techniques, shed light on the interaction mechanism of hydrogen with solid surfaces and reaction mechanisms in which hydrogen is involved. Future research challenges on neutron scattering studies of hydrides, as well as catalysis in general, are also highlighted, and more operando‐type neutron studies need be conducted to advance the field.

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Section: Hydrogen Interactions With Oxide Catalystsmentioning

confidence: 99%

Neutron Scattering Investigations of Hydride Species in Heterogeneous Catalysis

et al. 2018

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“…The resulting ex situ spectra unambiguously reveal the presence of hydrocarbon species, which may be associated with a hydrocarbon pool. Whereas O'Malley et al [28] concentrated on methanol exposure to ZSM-5 at room temperature, this communication describes an investigation performed at reaction temperatures representative of those utilised in MTG unit operations. Thus, INS is being used here to assess how hydrogen is partitioned within the catalyst matrix during conditions that correspond to the commercially relevant active phase of MTG operation.…”

Section: Introductionmentioning

confidence: 99%

“…Given the ability of INS to selectively probe hydrogeneous vibrational modes [15], it is enticing to discover whether the technique can provide new information on the adsorbed hydrocarbon species present at various stages of the methanol to hydrocarbon reaction. Very recently, O'Malley et al [28] have used a combination of neutron scattering methods matched by ab initio calculations to investigate, amongst other things, the reaction of methanol with ZSM-5 at room temperature. That study showed methanol to be immobilized due to methoxylation, and that the formation of adsorbed methoxy groups is facile over this material at room temperature.…”

Section: Introductionmentioning

confidence: 99%

Application of Inelastic Neutron Scattering to the Methanol-to-Gasoline Reaction Over a ZSM-5 Catalyst

et al. 2016

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Inelastic neutron scattering (INS) is used to investigate a ZSM-5 catalyst that has been exposed to methanol vapour at elevated temperature. In-line mass spectrometric analysis of the catalyst exit stream confirms methanol-to-gasoline chemistry, whilst ex situ INS measurements detect hydrocarbon species formed in/on the catalyst during methanol conversion. These preliminary studies demonstrate the capability of INS to complement infrared spectroscopic characterisation of the hydrocarbon pool present in/on ZSM-5 during the MTG reaction. Graphical Abstract& David Lennon

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“…[19] This technique has previously synergized well with other in situ characterization tools to better understand many catalytic processes. [20] We therefore present, for the first time, a combined in situ FTIR and QENS study on SAPO-34. We aim to integrate knowledge of the specific interactions of the reaction mechanism, with understanding of the structureproperty relationships, which dictate the diffusive motion of the organic moieties.…”

Section: Introductionmentioning

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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Room temperature methoxylation in zeolites: insight into a key step of the methanol-to-hydrocarbons process

Cited by 61 publications

References 46 publications

Neutron Scattering Investigations of Hydride Species in Heterogeneous Catalysis

Neutron Scattering Investigations of Hydride Species in Heterogeneous Catalysis

Application of Inelastic Neutron Scattering to the Methanol-to-Gasoline Reaction Over a ZSM-5 Catalyst

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

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