Cluster Model DFT Study of CO Adsorption to Gallium Ions in Ga/HZSM-5 | Sciact - CRIS-system of Boreskov Institute of Catalysis

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

Journal

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

Output data

Year: 2008, Volume: 112, Number: 9, Pages: 3321-3326 Pages count : 6 DOI: 10.1021/jp076379u

Tags

Adsorption; Density functional theory; Gallium compounds; Zeolites

Authors

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

Affiliations

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

Funding (2)

1	Russian Foundation for Basic Research	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 ANCAN OpenAlex

Submitted:	Aug 8, 2007
Accepted:	Dec 3, 2007
Published online:	Feb 12, 2008
Published print:	Mar 1, 2008

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

DB	Citing
Web of science	23
Scopus	24
Elibrary	22
OpenAlex	26