Preparation, Composition, Catalytic Properties of MFI-Type Zeolite Solid Solutions Hx[Al3+x Ti4+ySi4+12−x-yO24] with Al (x < 0.06) and Ti (y < 0.13) content | Sciact - CRIS-система Института катализа

Preparation, Composition, Catalytic Properties of MFI-Type Zeolite Solid Solutions Hx[Al3+x Ti4+ySi4+12−x-yO24] with Al (x < 0.06) and Ti (y < 0.13) content Научная публикация

Журнал

Journal of Porous Materials
ISSN: 1380-2224 , E-ISSN: 1573-4854

Вых. Данные

Год: 2025, DOI: 10.1007/s10934-025-01766-1

Ключевые слова

Zeolites; Crystal structure; X-ray diffraction (XRD); X-ray absorption spectroscopy; Catalytic properties

Авторы

Kuz’micheva Galina M. ¹ , Domoroshchina Elena N. ¹ , Kravchenko Galina V. ¹ , Chernyshev Vladimir V. ^2,3 , Khramov Evgeny V. ⁴ , Chumakov Ratibor G. ⁴ , Pavlov Ivan S. ⁵ , Vasil’ev Alexander L. ⁵ , Pirutko Larisa V. ⁶ , Kustov Alexander L. ^2,7 , Dorokhov Andrey A. ¹

Организации

1	MIREA-Russian Technological University, Moscow, Russia 119454
2	Department of Chemistry, Lomonosov Moscow State University, Moscow, Russia 119991
3	Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences, Moscow, Russia 119071
4	National Research Center “Kurchatov Institute”, Moscow, Russian Federation 123182
5	Shubnikov Institute of Crystallography of Federal Scientific Research Centre “Crystallography and Photonics” of Russian Academy of Sciences, Moscow, Russia 119333
6	Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, Russia 630090
7	Zelinsky Institute of Organic Chemistry, RAS, Moscow, Russia 119991

Информация о финансировании (2)

1	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	FWUR-2024-0035
2	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	075-15-2021-1362

For the first time, isomorphic substitution solid solutions of MFI-type zeolites (ZSM-5) Hx[Al3+x Ti4+ ySi4+12−x-yO24] (MFI-(Si,Al,Ti) were synthesized by hydrothermal method under the same conditions. A detailed characterization of the sample composition, the phase with the zeolite structure, the particle surface, as well as the crystal structure, the local structure of titanium and the microstructure was carried out using EDX, FTIR, DSC, XPS, EXAFS/XANES, S/TEM, BET, and BJH methods. It was established the difference between the initial compositions of solid solutions (Al ≤ 1.52 mol.% and Ti ≤ 4.28 mol.%) and the real one (Al ≤ 0.5 mol.% and Ti ≤ 1.0 mol.%) caused by the presence of anatase impurity phase or amorphous oxygen aluminum containing phase, uncontrolled potassium impurities in MFI-(Si,Al,Ti) samples and different amounts of molecules residues outside the framework (outside the square brackets) in the zeolite crystal structure with the formation of intercalated phases Hx[Al3+xTi4+ySi4+12−x-yO24] × wA (A = H2O and TPAOH). The established correlations between the individual characteristics of MFI-(Si,Al,Ti) with low Al and Ti content in the zeolite phase and their catalytic activity made it possible to find optimal MFI-(Si,Al,Ti) compositions for use as catalysts: maximum selectivity (97.1 and 97.9%) in the reaction of allyl chloride epoxidation to epichlorohydrin were achieved for samples with the highest Ti content in the zeolite phases and Ti3+ ions on MFI-(Si,Al,Ti) surface; in N2O decomposition reaction, maximum conversion value (52% at 650 °C) was obtained on MFI-(Si,Al,Ti) with an X-ray amorphous phase, maximum specific surface area, minimum content of Ti ions and a large Al content in the zeolite phase.

Kuz’micheva G.M. , Domoroshchina E.N. , Kravchenko G.V. , Chernyshev V.V. , Khramov E.V. , Chumakov R.G. , Pavlov I.S. , Vasil’ev A.L. , Pirutko L.V. , Kustov A.L. , Dorokhov A.A.
Preparation, Composition, Catalytic Properties of MFI-Type Zeolite Solid Solutions Hx[Al3+x Ti4+ySi4+12−x-yO24] with Al (x < 0.06) and Ti (y < 0.13) content
Journal of Porous Materials. 2025. DOI: 10.1007/s10934-025-01766-1 WOS Scopus OpenAlex

Опубликована online:

6 февр. 2025 г.

Web of science:	WOS:001415641500001
Scopus:	2-s2.0-85218038761
OpenAlex:	W4407218594

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