Cluster Model DFT Study of CO Adsorption to Gallium Ions in Ga/HZSM-5 | Sciact - CRIS-система Института катализа

Cluster Model DFT Study of CO Adsorption to Gallium Ions in Ga/HZSM-5 Научная публикация

Журнал

The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455

Вых. Данные

Год: 2008, Том: 112, Номер: 9, Страницы: 3321-3326 Страниц : 6 DOI: 10.1021/jp076379u

Ключевые слова

Adsorption; Density functional theory; Gallium compounds; Zeolites

Авторы

Zhidomirov George M. ¹ , Shubin Alexander A. ¹ , Milov M.A. ¹ , Kazanskii Vladimir B. ² , van Santen Rutger A. ³ , Hensen Emiel J.M. ³

Организации

1	Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Pr. Akad. Lavrentieva 5, Novosibirsk 630090, Russia
2	Zelinsky Institute of Organic Chemistry of Russian Academy of Sciences, Leninsky prospect 47, Moscow 117913, Russia
3	Schuit Institute of Catalysis, EindhoVen UniVersity of Technology, P.O. Box 513, 5600 MB, EindhoVen, The Netherlands

Информация о финансировании (2)

1	Российский фонд фундаментальных исследований	05-03-33103
2	Netherlands Organisation for Scientific Research	047-015-001

Cluster model DFT calculations of CO adsorption on various possible forms of gallium in Ga/HZSM-5 zeolites have been performed. CO was found to only weakly interact with Ga+, (GaO)+, and (Ga(OH)2-nHn)+ (n) 1, 2) cationic clusters. The resulting shifts of the CO stretching frequency (∆νCO) are only very small. On the other hand, CO coordination to small mononuclear and binuclear Ga3+ hydride/hydroxide/oxide species results in positive shifts in the stretching frequency in the range ∆νCO ) 20-40 cm-1. Larger shifts (∆νCO ) 70-90cm-1) are associated with CO coordination to Ga ions at the corners of small three-dimensional Ga-oxide clusters. The experimentally observed changes in the infrared spectrum of adsorbed CO over Ga/HZSM-5 zeolites upon reductive and oxidative treatments are interpreted with these insights. Possibilities for the formation of such polynuclear oxide species in the zeolite micropore space are discussed. On the basis of recent literature insights, we suggest that large shifts derive from CO coordination to oligomeric Ga cationic complexes stabilized by the negative zeolite charge.

Zhidomirov G.M. , Shubin A.A. , Milov M.A. , Kazanskii V.B. , van Santen R.A. , Hensen E.J.M.
Cluster Model DFT Study of CO Adsorption to Gallium Ions in Ga/HZSM-5
The Journal of Physical Chemistry C. 2008. V.112. N9. P.3321-3326. DOI: 10.1021/jp076379u WOS Scopus РИНЦ CAPlusCA OpenAlex

Поступила в редакцию:	8 авг. 2007 г.
Принята к публикации:	3 дек. 2007 г.
Опубликована online:	12 февр. 2008 г.
Опубликована в печати:	1 мар. 2008 г.

Web of science:	WOS:000253512400026
Scopus:	2-s2.0-41749101956
РИНЦ:	13580717
Chemical Abstracts:	2008:176394
Chemical Abstracts (print):	148:411537
OpenAlex:	W2128939016

БД	Цитирований
Web of science	21
Scopus	22
РИНЦ	20
OpenAlex	24