Catalytic properties and nature of active centers of ferrospheres in oxidative coupling of methane

被引:23
作者
Anshits, Alexander G. [1 ]
Bayukov, Oleg A. [1 ,2 ]
Kondratenko, Evgenii V. [3 ]
Anshits, Natalia N. [1 ]
Pletnev, Oleg N. [2 ]
Rabchevskii, Evgenii V. [1 ]
Solovyov, Leonid A. [1 ]
机构
[1] Russian Acad Sci, Siberian Branch, Inst Chem & Chem Technol, Akad Gorodok 50-24, Krasnoyarsk 660036, Russia
[2] Russian Acad Sci, Siberian Branch, Kirensky Inst Phys, Akad Gorodok 50-38, Krasnoyarsk 660036, Russia
[3] Univ Rostock, Leibniz Inst Katalyse eV, Albert Einstein Str 29 a, D-18059 Rostock, Germany
基金
俄罗斯科学基金会;
关键词
Methane coupling; Active center; Ferrospinel; Mossbauer spectroscopy; GLASS CRYSTAL CATALYSTS; MAGNETIC-PROPERTIES; PROFILE REFINEMENT; MOSSBAUER; PERFORMANCE; CONVERSION; ETHYLENE; MGO;
D O I
10.1016/j.apcata.2016.06.032
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ferrospheres with the Fe2O3 content in the range from 76 to 97 wt% were applied as catalysts for the oxidative coupling of methane (OCM). To identify their phase composition and distribution of iron sites, the ferrospheres were characterized by X-ray powder diffraction and Mossbauer spectroscopy before and after the OCM reaction. Magnetite-based ferrite spinel, hematite and aluminosilicate glasses were established to be the main phases. The ferrospinel of all ferrospheres partially oxidized to hematite after the OCM reaction. It was established that the yield of C-2-hydrocarbons sharply increased at the ferrospheres with Fe2O3 content higher than 89 wt% The spinel phase of these ferrospheres includes Fevv3+(B) sites with a Ca2+ tetrahedral cation and an octahedral cation vacancy among the nearest neighbors. A linear correlation between the yield of C-2-hydrocarbons (ethane and ethylene) and the content of such sites was established, thus indicating that their electrophilic oxygen species participate in selective CH4 conversion to C2H6. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:192 / 199
页数:8
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