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Impact of Composition and Structural Parameters on the Catalytic Activity of MFI Type Titanosilicalites Full article

Journal Dalton Transactions
ISSN: 1477-9226 , E-ISSN: 1477-9234
Output data Year: 2022, Volume: 51, Number: 9, Pages: 3439-3451 Pages count : 13 DOI: 10.1039/d1dt04131b
Tags C (programming language); Catalyst activity; Chlorine compounds; Fourier transform infrared spectroscopy; Ions; Nitrogen oxides; Nuclear magnetic resonance spectroscopy; Propane; Selective catalytic reduction; Silicates; Temperature programmed desorption; Titanium; X ray absorption spectroscopy; X ray powder diffraction
Authors Kuz'micheva Galina 1 , Chernyshev Vladimir 2,3 , Kravchenko Galina 1 , Pirutko Larisa 4 , Khramov Evgeny 5 , Bruk Lev 1 , Pastukhova Zhanna 1 , Kustov Aleksander 2,6 , Kustov Leonid 2,6 , Markova Ekaterina 7
Affiliations
1 MIREA-Russian Technological University, Moscow, 119454, Russia
2 Department of Chemistry, Lomonosov Moscow State University, Leninskie Gory 1-3, Moscow, 119991, Russia
3 Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences, Moscow, 119071, Russia
4 Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, 630090, Russia
5 National Research Center “Kurchatov Institute“, Moscow, 123182, Russia
6 N.D. Zelinsky Institute of Organic Chemistry, Moscow, 119991, Russia
7 Peoples Friendship University of Russia RUDN University, Moscow, 117198, Russia

Funding (2)

1 Ministry of Science and Higher Education of the Russian Federation 0706-2020-0026
2 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0006

Abstract: Titanosilicalite of the MFI type was obtained via a hydrothermal method. Its initial and annealed at 75 °C (TS-1P(75)) and 500 °C (TS-1P(500)) forms were studied by X-ray powder diffraction (PXRD), X-ray absorption spectroscopy (XAS-method), Fourier-transform infrared (FT-IR) spectroscopy, differential scanning calorimetry (DSC), temperature-programmed ammonia desorption (TPD NH3), and pyridine adsorption (Py). The full-profile Rietveld method allowed us to observe the presence of the organic template tetrapropylammonium hydroxide (TPAOH) in the framework voids, as well as to determine the silicate module (Si/Ti = 73.5) and the distribution of Ti4+ ions over the MFI-type structure sites (Ti atoms replace Si ones in two positions: T1 and T6). The coordination numbers of titanium (CNTi = 4.6 for TS-1P and TS-1P(75), CNTi = 3.8 for TS-1P(500)) were established by the XAS-method. The catalytic activity of titanosilicalites was found in the reactions of nitrous oxide decomposition (the maximal decomposition rate is demonstrated for the TS-1P(75) sample), allyl chloride epoxidation to epichlorohydrin (the best combination of all indicators was exhibited for the TS-1P sample) and propane conversion (maximum propane conversion, and butadiene and propylene selectivity were observed in both TS-1P(75) and TS-1P(500) samples). Mechanisms for the catalytic processes are proposed. The relationship between the catalytic properties and the composition (Si/Ti), Ti4+ ion distribution over the MFI-type structure sites, the local environment of titanium ions, and the number of acid sites in the titanosilicalites are discussed.
Cite: Kuz'micheva G. , Chernyshev V. , Kravchenko G. , Pirutko L. , Khramov E. , Bruk L. , Pastukhova Z. , Kustov A. , Kustov L. , Markova E.
Impact of Composition and Structural Parameters on the Catalytic Activity of MFI Type Titanosilicalites
Dalton Transactions. 2022. V.51. N9. P.3439-3451. DOI: 10.1039/d1dt04131b WOS Scopus РИНЦ ANCAN PMID OpenAlex
Dates:
Submitted: Dec 8, 2021
Accepted: Jan 28, 2022
Published online: Jan 31, 2022
Published print: Mar 7, 2022
Identifiers:
Web of science: WOS:000755248300001
Scopus: 2-s2.0-85125554652
Elibrary: 48187070
Chemical Abstracts: 2022:373396
Chemical Abstracts (print): 179:17606
PMID: 35167633
OpenAlex: W4210621010
Citing:
DB Citing
Web of science 4
Scopus 5
Elibrary 4
OpenAlex 8
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