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Nonstoichiometric Oxygen in Mn–Ga–O Spinels: Reduction Features of the Oxides and Their Catalytic Activity Full article

Journal RSC Advances
ISSN: 2046-2069
Output data Year: 2018, Volume: 8, Number: 21, Pages: 11598-11607 Pages count : 10 DOI: 10.1039/c7ra11557a
Tags THIN-FILMS; MANGANESE OXIDES; CO OXIDATION; NANOPARTICLES; TEMPERATURE; PERFORMANCE; COMBUSTION; MN2O3
Authors Bulavchenko O. A. 1,2 , Venediktova O. S. 1,2 , Afonasenko T. N. 3 , Tsyrul'nikov P. G. 3 , Saraev A. A. 1,2 , Kaichev V. V. 1,2 , Tsybulya S. V. 1,2
Affiliations
1 Boreskov Institute of Catalysis SB RAS, Lavrentieva Ave. 5, Novosibirsk, 630090, Russia
2 Novosibirsk State University, Pirogova Str. 2, Novosibirsk, 630090, Russia
3 Institute of Hydrocarbons Processing SB RAS, Neftezavodskaya Str. 54, Omsk, 644040, Russia

Funding (1)

1 Federal Agency for Scientific Organizations 0303-2016-0002

Abstract: The subject of this study was the content of oxygen in mixed oxides with the spinel structure Mn1.7Ga1.3O4 that were synthesized by coprecipitation and thermal treatment in argon at 600–1200 °C. The study revealed the presence of excess oxygen in “low-temperature” oxides synthesized at 600–800 °C. The occurrence of superstoichiometric oxygen in the structure of Mn1.7Ga1.3O4+δ oxide indicates the formation of cationic vacancies, which shows up as a decreased lattice parameter in comparison with “high-temperature” oxides synthesized at 1000–1200 °C; the additional negative charge is compensated by an increased content of Mn3+ cations according to XPS. The low-temperature oxides containing excess oxygen show a higher catalytic activity in CO oxidation as compared to the high-temperature oxides, the reaction temperature was 275 °C. For oxides prepared at 600 and 800 °C, catalytic activity was 0.0278 and 0.0048 cm3 (CO) per g per s, and further increase in synthesis temperature leads to a drop in activity to zero. The process of oxygen loss by Mn1.7Ga1.3O4+δ was studied in detail by TPR, in situ XRD and XPS. It was found that the hydrogen reduction of Mn1.7Ga1.3O4+δ proceeds in two steps. In the first step, excess oxygen is removed, Mn1.7Ga1.3O4+δ → Mn1.7Ga1.3O4. In the second step, Mn3+ cations are reduced to Mn2+ in the spinel structure with a release of manganese oxide as a single crystal phase, Mn1.7Ga1.3O4 → Mn2Ga1O4 + MnO.
Cite: Bulavchenko O.A. , Venediktova O.S. , Afonasenko T.N. , Tsyrul'nikov P.G. , Saraev A.A. , Kaichev V.V. , Tsybulya S.V.
Nonstoichiometric Oxygen in Mn–Ga–O Spinels: Reduction Features of the Oxides and Their Catalytic Activity
RSC Advances. 2018. V.8. N21. P.11598-11607. DOI: 10.1039/c7ra11557a WOS Scopus РИНЦ AN PMID OpenAlex
Files: Full text from publisher
Dates:
Submitted: Oct 19, 2017
Accepted: Mar 9, 2018
Published online: Mar 27, 2018
Identifiers:
Web of science: WOS:000428672500041
Scopus: 2-s2.0-85044627083
Elibrary: 35488796
Chemical Abstracts: 2018:602427
PMID: 35542767
OpenAlex: W2794568465
Citing:
DB Citing
Web of science 22
Scopus 23
Elibrary 21
OpenAlex 25
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