Guiding the design of practical MTW zeolite catalysts: An integrated experimental-theoretical perspective

Feng, Gang; Wen, Zhihui; Wang, Jiancheng; Lu, Zhang‐Hui; Zhou, Jian; Zhang, Rongbin

doi:10.1016/j.micromeso.2020.110810

Cited by 13 publications

(5 citation statements)

References 196 publications

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“…Compared to ZSM-12-Nano, ZSM-12-Con has a higher Si/Al ratio of 30.5. It should be noted that it is difficult to synthesize phase-pure ZSM-12 with a Si/Al ratio lower than 30 with MTEACl. , 27 Al NMR spectroscopy was used to investigate the chemical environment of the Al atoms in the zeolite samples. The corresponding spectra in Figure are dominated by main peaks at 53 and 56 ppm for EU-1 and ZSM-12 zeolites, respectively, corresponding to tetrahedrally coordinated framework Al (Al IV ).…”

Section: Resultsmentioning

confidence: 99%

Zeolite Nanocrystals (MOR, EU-1, and ZSM-12) Synthesized Using a Versatile Diquaternary Ammonium Template as Robust Catalysts

Liutkova

Hensen

2022

ACS Appl. Nano Mater.

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Nanocrystals of zeolites with shortened diffusional pathways compared to bulk counterparts are attractive catalysts, but their direct synthesis often remains challenging and expensive. Here, we describe the utility of p-phenylenedimethylene−bis(trimethylammonium) dichloride, an organic diquaternary ammonium compound that can be easily prepared, as an effective organic structuredirecting agent (OSDA) for obtaining several zeolites composed of agglomerated nanocrystals. By modifying the gel composition (NaOH/ Si and Si/Al ratios) and crystallization time, synthesis can be tuned to obtain mordenite, EU-1, and ZSM-12 zeolites. 13 C NMR spectra of the occluded OSDA reveal subtle differences in host−guest interactions between the OSDA and the respective zeolites, which derives from the flexibility of the OSDA. The relatively strong interaction between the OSDA and inorganic aluminosilicate precursor species during the induction period explains how small zeolite nanocrystals are obtained. Nanosized EU-1 and ZSM-12 significantly outperform their corresponding bulk counterparts as acid catalysts in the methanol-to-hydrocarbons reaction and the alkylation of benzene with benzyl alcohol, respectively.

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Section: Resultsmentioning

confidence: 99%

Zeolite Nanocrystals (MOR, EU-1, and ZSM-12) Synthesized Using a Versatile Diquaternary Ammonium Template as Robust Catalysts

Liutkova

Hensen

2022

ACS Appl. Nano Mater.

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“…Tetravalent metal ions (Ti 4+ , Ge 4+ , Zr 4+ , Sn 4+ ) can be incorporated into the zeolite by means of isomorphous substitution to introduce the well-defined Lewis acid center for the zeolite, which can enhance the catalytic activity of the zeolite for a designated reaction. − Mal et al reported Sn-ZSM-12 zeolite with a Si/Sn >70 that could be used as an effective catalyst for the oxidation of phenol, m -cresol, and m -xylene, which performed better than the Sn-free ZSM-12. They also found that Sn-ZSM-12 exhibited better activity than mesoporous Sn-MFI/MEL in the oxidation of naphthalene and 2-methylnaphthalene to naphthol, 2-naphthalenemethanol and 2-naphthaldehyde .…”

Section: Introductionmentioning

confidence: 99%

Comparative First-Principles Study on Tetravalent Ion-Incorporated MTW-Type Zeolites

Jin

Zhang

et al. 2023

J. Phys. Chem. C

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The density functional theory (DFT) with dispersion correction was used to study the tetravalent metal (Ti, Zr, Ge, Sn)-incorporated MTW-type (Mobil-TWelve) zeolites that are usually denoted as ZSM-12 (Zeolite Socony Mobil-twelve). Their stability, Lewis acidity, and structural properties were analyzed with periodic models. The calculated substitution energies indicate that Ti and Zr are more easily incorporated into MTW than Ge and Sn. The most stable substitution energies of four elements correlate with their covalent radii (R 2 = 0.95), implying that the thermodynamics of incorporation process could be designed by covalent radii. Incorporations of a tetravalent metal result in the variation of cell volume due to their larger covalent radii; significantly, there is a good correlation between substitution energies and cell volume, indicating that the stability could be judged by the cell volume from accessible characterization. The Lewis acidity is measured by ammonia adsorption as follows: Sn-MTW > Zr-MTW > Ti-MTW > Ge-MTW. This finding provides the basis of theoretical Lewis acidity and agrees with previous experiments. In addition, the structural deformation has a great influence on the zeolitic stability, proved by two correlations: (1) relative mean square deviation of [MO4] and substitution energy of Ti-, Ge-, and Sn-MTW and (2) root-mean-square error of [MSi4] and substitution energy of Zr-MTW. Our work provides the theoretical basis for the preparation and Lewis acidity of tetravalent metal-incorporated MTW-type zeolitic catalysts.

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“…In the present study, we aimed to compare the activity of zeolite-based Cu catalysts for plasma-catalytic dry methane reforming. A zeolite of the MTW (ZSM-12) type was chosen for comparison with the widely used MFI (ZSM-5) zeolite due to its unique porous structure and tuning acidity availability [41]. To the best of our knowledge, the MTW-type zeolite was not studied in plasma-catalytic dry methane reforming so far by other researchers.…”

Section: Introductionmentioning

confidence: 99%

Greenhouse Gas Conversion into Hydrocarbons and Oxygenates Using Low Temperature Barrier Discharge Plasma Combined with Zeolite Catalysts

Golubev,

Tsaplin,

Maximov

2023

Gases

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Global warming occurs as a result of the build-up of greenhouse gases in the atmosphere, causing an increase in Earth’s average temperature. Two major greenhouse gases (CH4 and CO2) can be simultaneously converted into value-added chemicals and fuels thereby decreasing their negative impact on the climate. In the present work, we used a plasma-catalytic approach for the conversion of methane and carbon dioxide into syngas, hydrocarbons, and oxygenates. For this purpose, CuCe zeolite-containing catalysts were prepared and characterized (low-temperature N2 adsorption, XRF, XRD, CO2-TPD, NH3-TPD, TPR). The process of carbon dioxide methane reforming was conducted in a dielectric barrier discharge under atmospheric pressure and at low temperature (under 120 °C). It was found that under the studied conditions, the major byproducts of CH4 reforming are CO, H2, and C2H6 with the additional formation of methanol and acetone. The application of a ZSM-12 based catalyst was beneficial as the CH4 conversion increased and the total concentration of liquid products was the highest, which is related to the acidic properties of the catalyst.

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Guiding the design of practical MTW zeolite catalysts: An integrated experimental-theoretical perspective

Cited by 13 publications

References 196 publications

Zeolite Nanocrystals (MOR, EU-1, and ZSM-12) Synthesized Using a Versatile Diquaternary Ammonium Template as Robust Catalysts

Zeolite Nanocrystals (MOR, EU-1, and ZSM-12) Synthesized Using a Versatile Diquaternary Ammonium Template as Robust Catalysts

Comparative First-Principles Study on Tetravalent Ion-Incorporated MTW-Type Zeolites

Greenhouse Gas Conversion into Hydrocarbons and Oxygenates Using Low Temperature Barrier Discharge Plasma Combined with Zeolite Catalysts

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