Insights into the Site-Selective Adsorption of Methanol and Water in Mordenite Zeolite by <sup>129</sup>Xe NMR Spectroscopy

Gong, Kecheng; Jiao, Feng; Chen, Yuxiang; Liu, Xianchun; Pan, Xiulian; Han, Xiuwen; Bao, Xinhe; Hou, Guangjin

doi:10.1021/acs.jpcc.9b04350

Cited by 10 publications

(7 citation statements)

References 34 publications

(60 reference statements)

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“…In our recent studies, we found that the hybrid OX/ZEO catalyst consisting of MOR and ZnCrO x showed extremely high ethylene selectivity for syngas conversion, and it was attributed to the BAS within the 8MR side pockets of MOR via a ketene intermediate . It is also found that the BASs in dual pores of MOR possess distinct selective adsorptions for guest molecules or intermediate molecules …”

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confidence: 97%

“…4 It is also found that the BASs in dual pores of MOR possess distinct selective adsorptions for guest molecules or intermediate molecules. 11 A variety of methods including X-ray diffraction (XRD), 12 Fourier-transform infrared (FTIR) spectroscopy, 13,14 quantum chemical calculations, 15,16 and nuclear magnetic resonance (NMR) 17,18 have been employed to study the location of BASs in H-type mordenite (H-MOR). Specifically, Mortier et al studied dehydrated H-MOR by XRD and concluded that there was no convincing evidence for preferential attachment of protons to any particular framework oxygen.…”

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confidence: 99%

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Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Gong

Liu

et al. 2021

J. Phys. Chem. Lett.

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Herein, utilizing acetonitrile as the probe molecule, the acidity and host–guest interactions of H-mordenite (H-MOR) zeolites are investigated comprehensively by solid-state NMR spectroscopy and theoretical calculation. The locations and local configurations of Brønsted acid sites (BASs) in H-MOR are revealed by multinuclear and multidimensional NMR experiments with adsorption/coadsorption of acetonitrile (CD3CN) and trimethylphosphine (TMP). Moreover, the confinement effect of dual pores in MOR has been characterized via the quantitative determination of host–guest interactions between CH3CN and BASs. The 1H–15N dipolar measurement results and DFT calculations demonstrate that there are two kinds of acetonitrile molecules adsorbed in 12-membered ring (12MR) main channels with distinct mobility, where acetonitrile undergoes either partially restricted or highly flexible motion in the time scale of nanoseconds to microseconds. These two types of acetonitrile can exchange with temperature rising. In contrast, the mobility of acetonitrile in 8-membered ring (8MR) channels is very restricted due to the confinement of the framework.

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confidence: 97%

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confidence: 99%

Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Gong

Liu

et al. 2021

J. Phys. Chem. Lett.

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“…( 1 )), while the formed water molecules are not released easily from the zeolite structure and hence hinder zeolite activity by formation of strong interactions with the BAS. Thus, MeOH dehydration ultimately inhibits the formation of SMS 32 , 33 . …”

Section: Resultsmentioning

confidence: 99%

Charge-separation driven mechanism via acylium ion intermediate migration during catalytic carbonylation in mordenite zeolite

Chen

Tarach

et al. 2022

Nat Commun

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By employing ab initio molecular dynamic simulations, solid-state NMR spectroscopy, and two-dimensional correlation analysis of rapid scan Fourier transform infrared spectroscopy data, a new pathway is proposed for the formation of methyl acetate (MA) via the acylium ion (i.e.,CH3 − C ≡ O+) in 12-membered ring (MR) channel of mordenite by an integrated reaction/diffusion kinetics model, and this route is kinetically and thermodynamically more favorable than the traditional viewpoint in 8MR channel. From perspective of the complete catalytic cycle, the separation of these two reaction zones, i.e., the C-C bond coupling in 8MR channel and MA formation in 12MR channel, effectively avoids aggregation of highly active acetyl species or ketene, thereby reducing undesired carbon deposit production. The synergistic effect of different channels appears to account for the high carbonylation activity in mordenite that has thus far not been fully explained, and this paradigm may rationalize the observed catalytic activity of other reactions.

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“…Moreover, the rate‐controlled mercury penetration method was used to analyse the pore‐throat radius of different types of tight sandstones and the correlation between the pore‐throat radius and the physical properties of reservoirs, in order to determine the impacts of pore‐throat radius on the reservoir permeability. The NMR is a useful tool for analysing the characteristics of pore fluids in reservoirs, especially for determining the movable and irreducible water saturation (Gong et al, 2019; Peng, Zhang, Ma, & Pan, 2019). The NMR T2 spectrum was analysed to determine the movable fluid saturation of samples with different physical properties in the study area and to further define the pattern of different porosity and permeability varying with the movable fluid saturation.…”

Section: Samples and Methodsmentioning

confidence: 99%

Pore structure and reservoir physical properties for effective development of tight sandstone gas: A case study from the Central Sichuan Basin, China

et al. 2022

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Several large gas fields have been found in the Central Sichuan Basin in recent years, with proven reserves of more than 100 × 10 9 m3. Among these, the tight sandstone gas in the Late Triassic Xujiahe Formation is a key target in the Sichuan Basin. The key to the discovery of high‐yield areas rich in tight sandstone gas is to determine the pore structures and the lower limits of effective physical properties of reservoirs that control natural gas accumulation. In this study, we investigate the Late Triassic second Member of the Xujiahe Formation (hereinafter referred to as the Xu2 Member) in the Central Sichuan Basin as an example. We analyse the distribution characteristics of pores and throats in the reservoirs and identify that the reservoir in the study area is mainly characterized by small pores and narrow throats. The physical properties of reservoirs in the area are mainly controlled by pore‐throat radius and the permeability–porosity ratio. Nuclear magnetic resonance analysis indicates that the irreducible water saturation is mostly more than 50% and is inversely correlated with the physical properties of reservoirs in the study area. Meanwhile, with an increase in the physical properties of reservoirs, the proportion of large pores increases and the irreducible water saturation rapidly decreases. According to the gas–water two‐phase seepage experiment, for reservoirs with good physical properties, the gas relative permeability significantly increases with an increase in gas saturation and the reservoir permeability has more significant effects. Where the reservoir permeability is less than 0.4 mD, the permeability of both gas phase and water phases is only less than 0.1, and the mobility of both gas and water is poor. Only when the reservoir permeability is more than 0.4 mD, can the gas relative permeability reach more than 0.3, and the water mobility is significantly inhibited. In this case, favourable results can be achieved from the natural gas development. As verified by the development of the tight sandstone reservoirs in the Xu2 Member in Central Sichuan Basin, the lower limits of physical properties allowing for effective natural gas development include the reservoir permeability of more than 0.1 mD (preferably more than 0.2 mD) and the reservoir porosity of greater than 6%–7%.

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Insights into the Site-Selective Adsorption of Methanol and Water in Mordenite Zeolite by ¹²⁹Xe NMR Spectroscopy

Cited by 10 publications

References 34 publications

Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Charge-separation driven mechanism via acylium ion intermediate migration during catalytic carbonylation in mordenite zeolite

Pore structure and reservoir physical properties for effective development of tight sandstone gas: A case study from the Central Sichuan Basin, China

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Insights into the Site-Selective Adsorption of Methanol and Water in Mordenite Zeolite by 129Xe NMR Spectroscopy

Cited by 10 publications

References 34 publications

Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Acidity and Local Confinement Effect in Mordenite Probed by Solid-State NMR Spectroscopy

Charge-separation driven mechanism via acylium ion intermediate migration during catalytic carbonylation in mordenite zeolite

Pore structure and reservoir physical properties for effective development of tight sandstone gas: A case study from the Central Sichuan Basin, China

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Insights into the Site-Selective Adsorption of Methanol and Water in Mordenite Zeolite by ¹²⁹Xe NMR Spectroscopy