Fabrication of Hollow Mesoporous Nanosized ZSM‐5 Catalyst with Superior Methanol‐to‐Hydrocarbons Performance by Controllable Desilication

Fu, Tingjun; Qi, Ruiyue; Wan, Weili; Shao, Juan; Wen, John Z.; Li, Zhong

doi:10.1002/cctc.201700925

Cited by 27 publications

(15 citation statements)

References 54 publications

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“…It has been repeatedly proved that within agglomerated catalysts based on H‐ZSM‐5 zeolite having a mesoporous matrix, the growth rate of coke II is limited by the micropore topology of the H‐ZSM‐5 zeolite, whereas that of coke I is less limited. This has been confirmed in hierarchical zeolites too . This effect is due to the fact that in the disordered meso‐ and macropores of the matrix the growth of coke has less steric hindrance.…”

Section: Resultsmentioning

confidence: 62%

“…This has been confirmed in hierarchical zeolites too. [63] This effect is due to the fact that in the disordered meso-and macropores of the matrix the growth of coke has less steric hindrance. Furthermore, the presence of water in the MTH and DTH reactions regulates the capability of the acid sites to condensate HCP aromatics into coke, by sweeping out coke precursors.…”

Section: In-situ Ftir Spectroscopymentioning

confidence: 99%

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Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons

et al. 2019

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The conversions into hydrocarbons of methanol, dimethyl ether and chloromethane (MTH, DTH and CTH, respectively) on a H‐ZSM‐5 zeolite catalyst were compared trough ab‐initio calculations and experiments, using a fixed‐bed reactor and in‐situ FTIR spectroscopy. The molecular modelling of the reaction was performed using force field calculations. The nature and location of retained species were assessed by a combination of techniques. The experimental results of activity, product distribution and deactivation match these of the molecular modelling as the three reactions proceed through the dual‐cycle mechanism. However, the initiation, evolution and degradation of hydrocarbon pool species are kinetically different depending on the reactant. The reactions are faster in the order DTH>MTH≫CTH whereas the rate at which coke forms and grows (linked with the rate of deactivation) is in the order CTH≫DTH>MTH.

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Section: Resultsmentioning

confidence: 62%

Section: In-situ Ftir Spectroscopymentioning

confidence: 99%

Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons

et al. 2019

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“…However, the catalytic applications of ZSM‐5 zeolites are limited by mass transport in the microporous network if bulky molecules are involved in the reaction . In this regard, the introduction of mesopores into microporous zeolites to obtain hierarchical ones, possessing the catalytic features of microporosity and the improved mass transport consequence of mesoporosity, would be an optimal choice for better performance …”

Section: Introductionmentioning

confidence: 99%

“…[7,8] However,t he catalytic applications of ZSM-5 zeolitesa re limited by mass transport in the microporous network if bulky molecules are involved in the reaction. [9][10][11][12][13] In this regard,t he introduction of mesopores into microporous zeolites to obtain hierarchical ones,p ossessing the catalytic features of microporosity andt he improved mass transport consequence of mesoporosity, [14][15][16][17][18][19][20] would be an optimal choice for better performance. [21][22][23][24][25] Generally,t he acidic properties and the pore structure of hierarchical zeolites are the two main factorst od etermine the catalytic performance duringr eactions.…”

Section: Introductionmentioning

confidence: 99%

The Role of External Acidity of Hierarchical ZSM‐5 Zeolites in n‐Heptane Catalytic Cracking

et al. 2018

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The hierarchical ZSM‐5 zeolite, which contains mesopores in addition to intrinsic micropores, is expected to enhance the bulky molecular diffusion and accessibility of acid sites. These sites, distributed in the internal surface (micropore) or external environment (including external surface and mesopore walls), play different roles in chemical reactions. To explore the effect of internal/external acidity on the reaction, in this study, a series of hierarchical ZSM‐5 zeolites with similar pore structures but different external acid properties were synthesized. Tartaric acid was employed to poison the acidic sites in the external environment selectively and extract Al from the framework. The catalytic cracking of n‐heptane (the main compound of naphtha) was chosen as a model reaction. The results show that elimination of external active sites tends to reduce the coke formation. The more external acid sites are selectively eliminated, the better catalytic performance can be achieved because of suppressing the bimolecular reactions of ethylene and propylene.

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“…Unlike, NaY zeolite, the alkalitreated ZSM-5 zeolite with a relatively high Si/Al ratio resulted in the formation of mesopores and a hollow structure more easily because of the rich Al exterior area and also the gradient distribution of the Al content. 30,31…”

Section: Textural Properties Of the Supportsmentioning

confidence: 99%

Evolution of the pore and framework structure of NaY zeolite during alkali treatment and its effect on methanol oxidative carbonylation over a CuY catalyst

Yan

Wang

et al. 2020

Journal of Chemical Research

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Alkali treatment is widely used on aluminosilicate zeolites with high Si/Al ratios in order to fabricate mesopores in the framework. However, for zeolites with low Si/Al ratios, the effect of alkali treatment on the pore and framework structure needed further study. In this work, Y zeolite is treated with NaOH solutions of different concentrations and is used as the support for Cu-based catalysts for oxidative carbonylation of methanol to dimethyl carbonate. The physicochemical properties of the supports and corresponding catalysts are characterized by N2 adsorption–desorption, X-ray diffraction, X-ray fluorescence, transmission electron microscopy, inductively coupled plasma mass spectrometry, X-ray photoelectron spectroscopy, and H2-temperature-programmed reduction analyses. The results show that no obvious mesopores are formed under alkali treatment, even at high NaOH concentration. However, amorphous species present in the micropores of Y zeolite are removed, which increases the micropore surface area as well as the crystallinity. Simultaneously, the cage structure is partially destroyed, which also leads to a slight increase of the pore volume and surface area. The altered micropore structure eventually increases the content and accessibility of the exchanged Cu species, which is beneficial to the catalytic activity. When the concentration of NaOH is 0.6 M, the space time yield of dimethyl carbonate for the corresponding catalyst was 151.4 mg g−1 h−1 which is 3.3-fold higher than that of the untreated-Y-zeolite-supported Cu catalyst. However, further increasing the alkali treatment strength can seriously destroy the basic aluminosilicate structure of the Y zeolite and decrease its intrinsic ion-exchange capacity. This results in the formation of agglomerated CuO on the catalyst surface, which was not conducive to catalytic activity.

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Fabrication of Hollow Mesoporous Nanosized ZSM‐5 Catalyst with Superior Methanol‐to‐Hydrocarbons Performance by Controllable Desilication

Cited by 27 publications

References 54 publications

Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons

Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons

The Role of External Acidity of Hierarchical ZSM‐5 Zeolites in n‐Heptane Catalytic Cracking

Evolution of the pore and framework structure of NaY zeolite during alkali treatment and its effect on methanol oxidative carbonylation over a CuY catalyst

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