Al and Ti Location in the MFI Orthorhombic HZSM-5 Framework. DFT Calculation and Neutron Diffraction Experiment | Sciact - CRIS-система Института катализа

Al and Ti Location in the MFI Orthorhombic HZSM-5 Framework. DFT Calculation and Neutron Diffraction Experiment Научная публикация

Журнал

Journal of Materials Science
ISSN: 0022-2461 , E-ISSN: 1573-4803

Вых. Данные

Год: 2023, Том: 58, Страницы: 3934–3946 Страниц : 13 DOI: 10.1007/s10853-023-08294-w

Ключевые слова

Aluminum; Catalyst activity; Crystal atomic structure; Ions; Neutron diffraction; Silicon; Titanium; Zeolites

Авторы

Domoroshchina Elena N. ¹ , Svetogorov Roman D. ² , Kuz’micheva Galina M. ¹ , Kravchenko Galina V. ¹ , Pirutko Larisa V. ³ , Zhukova Anna I. ⁴ , Utenyshev Andrey N. ⁵ , Bozhenko Konstantin V. ^4,5

Организации

1	MIREA-Russian Technological University (RTU MIREA), 78 Vernadsky Avenue, Moscow, Russia, 119454
2	National Research Center “Kurchatov Institute”, 1, Akademika Kurchatova Pl, Moscow, Russia, 123182
3	Boreskov Institute of Catalysis, Siberian Branch, 5, Lavrentiev Ave, Novosibirsk, Russia, 630090
4	Friendship University of Russia (RUDN University), 6, Miklukho-Maklaya Str, Moscow, Russia, 117198
5	Institute of Problems of Chemical Physics, Russian Academy of Sciences, 1, Acad. Semenov av, Chernogolovka, Russia, 142432

Информация о финансировании (2)

1	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	0706-2020-0026
2	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	0089-2019-0013 (АААА-А19-119092390076-7)

For the first time the neutron diffraction study of HZSM-5 zeolites with the general composition of (H1+x)[Al3+xSi4+12-xO24] × wH2O in the orthorhombic approximation (sp. gr. Pnma, z = 8) and initial silicate modules Si/Al = 12, 25, 40 was carried out. As a result, the composition was refined, the distribution of Al3+ ions over the tetrahedral sites (T sites) of the structure was found, and their content in each of them was estimated. It was found that T sites occupation in HZSM-5 structure differ depending on Si/Al, while samples with the same silicate module (Si/Al = 40) obtained under different synthesis conditions differ in the distribution of Al3+ ions over T sites of the structure. It was shown that the calculation of HZSM-5 zeolites crystal structure with substitutions in T sites performed using the VASP 5.2 program with different optimizations (atomic coordinates and unit cell parameters) can only reveal the most thermodynamically energetically favorable sites for Si4+ atoms substitution with other atoms (aluminum and titanium) without predicting their content in each site and regardless zeolite synthesis conditions and type of substituent atom. The relationship between HZSM-5 zeolites catalytic properties and silicate module (Si/Al, Si/Ti) was found and it cannot be ruled out that HZSM-5 catalytic activity is related to Ti4+ ions distribution over the tetrahedral sites of the structure.

Domoroshchina E.N. , Svetogorov R.D. , Kuz’micheva G.M. , Kravchenko G.V. , Pirutko L.V. , Zhukova A.I. , Utenyshev A.N. , Bozhenko K.V.
Al and Ti Location in the MFI Orthorhombic HZSM-5 Framework. DFT Calculation and Neutron Diffraction Experiment
Journal of Materials Science. 2023. V.58. P.3934–3946. DOI: 10.1007/s10853-023-08294-w WOS Scopus РИНЦ CAPlusCA OpenAlex

Поступила в редакцию:	7 сент. 2022 г.
Принята к публикации:	7 февр. 2023 г.
Опубликована online:	21 февр. 2023 г.
Опубликована в печати:	1 мар. 2023 г.

Web of science:	WOS:000936228900004
Scopus:	2-s2.0-85148431578
РИНЦ:	54798408
Chemical Abstracts:	2023:365602
Chemical Abstracts (print):	182:122939
OpenAlex:	W4321437741

БД	Цитирований
Scopus	2
Web of science	4
OpenAlex	5
РИНЦ	4