Liquid-Phase Hydrogenation of 1-Phenyl-1-propyne on the Pd1Ag3/Al2O3 Single-Atom Alloy Catalyst: Kinetic Modeling and the Reaction Mechanism | Sciact - CRIS-система Института катализа

Liquid-Phase Hydrogenation of 1-Phenyl-1-propyne on the Pd1Ag3/Al2O3 Single-Atom Alloy Catalyst: Kinetic Modeling and the Reaction Mechanism Научная публикация

Журнал

Nanomaterials
, E-ISSN: 2079-4991

Вых. Данные

Год: 2021, Том: 11, Номер: 12, Номер статьи : 3286, Страниц : 23 DOI: 10.3390/nano11123286

Ключевые слова

single-atom alloy catalyst; alkyne; alkene selectivity; hydrogenation; 1-phenyl-1-propyne; kinetic modeling

Авторы

Rassolov Alexander V. ¹ , Mashkovsky Igor S. ¹ , Baeva Galina N. ¹ , Bragina Galina O. ¹ , Smirnova Nadezhda S. ¹ , Markov Pavel V. ¹ , Bukhtiyarov Andrey V. ² , Wärnå Johan ³ , Stakheev Alexander Yu. ¹ , Murzin Dmitry Yu. ³

Организации

1	N.D. Zelinsky Institute of Organic Chemistry RAS, Leninsky Prospect 47, 119991 Moscow, Russia
2	Synchrotron Radiation Facility SKIF, Boreskov Institute of Catalysis SB RAS, Nikol’skiy Prospekt 1, 630559 Kol’tsovo, Russia
3	Laboratory of Industrial Chemistry and Reaction Engineering, Faculty of Science and Engineering, Åbo Akademi University, FI-20500 Turku, Finland

Информация о финансировании (2)

1	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	ГЗ-2021-2023
2	Российский научный фонд	17-13-01526 (АААА-А17-117051110178-3)

This research was focused on studying the performance of the Pd1Ag3/Al2O3 single-atom alloy (SAA) in the liquid-phase hydrogenation of di-substituted alkyne (1-phenyl-1-propyne), and development of a kinetic model adequately describing the reaction kinetic being also consistent with the reaction mechanism suggested for alkyne hydrogenation on SAA catalysts. Formation of the SAA structure on the surface of PdAg3 nanoparticles was confirmed by DRIFTS-CO, revealing the presence of single-atom Pd1 sites surrounded by Ag atoms (characteristic symmetrical band at 2046 cm−1) and almost complete absence of multiatomic Pdn surface sites (<0.2%). The catalyst demonstrated excellent selectivity in alkyne formation (95–97%), which is essentially independent of P(H2) and alkyne concentration. It is remarkable that selectivity remains almost constant upon variation of 1-phenyl-1-propyne (1-Ph-1-Pr) conversion from 5 to 95–98%, which indicates that a direct alkyne to alkane hydrogenation is negligible over Pd1Ag3 catalyst. The kinetics of 1-phenyl-1-propyne hydrogenation on Pd1Ag3/Al2O3 was adequately described by the Langmuir-Hinshelwood type of model developed on the basis of the reaction mechanism, which suggests competitive H2 and alkyne/alkene adsorption on single atom Pd1 centers surrounded by inactive Ag atoms. The model is capable to describe kinetic characteristics of 1-phenyl-1-propyne hydrogenation on SAA Pd1Ag3/Al2O3 catalyst with the excellent explanation degree (98.9%).

Rassolov A.V. , Mashkovsky I.S. , Baeva G.N. , Bragina G.O. , Smirnova N.S. , Markov P.V. , Bukhtiyarov A.V. , Wärnå J. , Stakheev A.Y. , Murzin D.Y.
Liquid-Phase Hydrogenation of 1-Phenyl-1-propyne on the Pd1Ag3/Al2O3 Single-Atom Alloy Catalyst: Kinetic Modeling and the Reaction Mechanism
Nanomaterials. 2021. V.11. N12. 3286 :1-23. DOI: 10.3390/nano11123286 WOS Scopus РИНЦ CAPlus PMID OpenAlex СКИФ ID

Поступила в редакцию:	31 окт. 2021 г.
Принята к публикации:	29 нояб. 2021 г.
Опубликована в печати:	3 дек. 2021 г.
Опубликована online:	3 дек. 2021 г.

Web of science:	WOS:000736425200001
Scopus:	2-s2.0-85120623939
РИНЦ:	47536246
Chemical Abstracts:	2022:92030
PMID (PubMed):	34947637
OpenAlex:	W4200419458
СКИФ ID:	963

БД	Цитирований
Scopus	15
Web of science	14
РИНЦ	13
OpenAlex	15