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2013/3
Promotion and Alkaline Treatment of Type MFI Zeolite: Influence on Structure, Acidic Properties and Selectivity in Propane-Butane Conversion
Oil and gas processing, chemistry of oil and gas

Authors: Alexei G. DEDOV graduated from the Chemistry Department of Lomonosov Moscow State University in 1977. He is Corresponding Member of the Russian Academy of Sciences, Head of the Department of General and Inorganic Chemistry Gubkin Russian State University of Oil and Gas. He specializes in the field of catalysis and analytical chemistry, transformations of light alkanes. He is author of over 200 scientific publications. E-mail: genchem@gubkin.ru
Daria A. LEVCHENKO graduated from Gubkin Russian State University of Oil and Gas in 2010. She is graduate student of the Department of General and Inorganic Chemistry of Gubkin Russian State University of Oil and Gas, specializing in the field of catalytic transformations of hydrocarbons. E-mail: genchem@gubkin.ru
Nikolai A. SPESIVTSEV graduated from Kuban State Technological University in 2012. He is graduate student of the Department of General and Inorganic Chemistry of Gubkin Russian State University of Oil and Gas. He specializes in the field of X-ray diffraction. E-mail: genchem@gubkin.ru
Alexey S. LOKTEV graduated from the Chemistry Department of Lomonosov Moscow State University in 1979. He is Doctor of Chemical Sciences, Professor of the Department of General and Inorganic Chemistry of Gubkin Russian State University of Oil and Gas. He is a specialist in the field of catalysis, author of over 100 scientific publications. E-mail: genchem@gubkin.ru
Ayrat V. ISHMURZIN graduated from Kazan State Technical University in 1995. He is Candidate of Chemical Sciences, Head of the Department for Processing of Gas, Gas Condensate and Oil of JSC “Gazprom”. He is an expert in the field of refining and petrochemicals. E-mail: A.Ishmurzin@adm.gazprom.ru
Ilya I. MOISEEV graduated from Lomonosov Moscow Institute of Chemical Engineering in 1952. He is Full Member of the Russian Academy of Sciences, Professor of the Department of General and Inorganic Chemistry of Gubkin Russian State University of Oil and Gas. He is a specialist in the field of coordination chemistry and catalysis. He is author of over 600 scientific publications. E-mail: genchem@gubkin.ru

Abstract: The effect of the promotion with zinc and chromium, as well as treatment with NaOH solution of the structure, acid and catalytic properties of type MFI zeolite is studied. It is shown that the crystal structure of the zeolite remains unchanged after the introduction of promoters, alkaline treatment and use in the conversion of propane and butane fraction (PBF). At the same time, the promotion decreases the total acidity and the amount of strongly acidic centers accompanied by increased selectivity of aromatic hydrocarbons formation. After alkaline treatment the selectivity of aromatic hydrocarbons formation also increases, while the force of distribution of acid sites on the zeolite remains unchanged.

Index UDK: 665.656.6(043)

Keywords: catalysis, type MFI zeolite, structure, acidic properties, promotion with zinc and chromium, alkali treatment, propane-butane fraction, X-ray diffraction, thermo-sorption of ammonia

Bibliography:
1. Martinez A., Peris E., Derewinski M., Burkat-Dulak A. Improvement of catalyst stability during methane dehydroaromatization (MDA) on Mo/HZSM-5 comprising intracrystalline mesopores. Catalysis Today, 2011, vol. 169, p. 75–84.
2.
Frey K., Lubango L.M., Scurrell M.S., Guczi L. Light alkane aromatization over modified Zn-ZSM-5 catalysts: characterization of the catalysts by hydrogen/deuterium isotope exchange. Reaction Kinetics, Mechanisms and Catalysis, 2011, vol. 104, p. 303-309.
3.
Luzgin M.V., Gabrienko A.A., Rogov V.A., Toktarev A.V., Parmon V.N., Stepanov A.G. The “Alkyl” and “Carbenium” Pathways of Methane Activation on Ga-Modified Zeolite BEA: 13C Solid-State NMR and GC-MS Study of Methane Aromatization in the Presence of Higher Alkane. Journal of Physical Chemistry C., 2010, vol. 114, p. 21555–21561.
4.
Stepanov A.G., Arzumanov S.S., Gabrienko A.A., Parmon V.N., Ivanova I.I., Freude D. Significant Influence of Zn on Activation of the C-H Bonds of Small Alkanes by Broensted Acid Sites of Zeolite. ChemPhysChem, 2008, vol. 9, p. 2559-2563.
5.
Gabrienko A.A., Arzumanov S.S., Freude D., Stepanov A.G. Propane Aromatization on Zn-Modified Zeolite BEA Studied by Solid-State NMR in Situ. Journal of Physical Chemistry C., 2010, vol. 114, p. 12681–12688.
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Baerlocher C., McCusker L. B., Olson D. H. Atlas of Zeolite Framework Types. 6th ed. New York: Elsevier Inc., 2007, 398 p.
7. Additivnoe vlijanie oksidov hroma i cinka na aktivnost’ ceolita marki NCVM v aromatizacii propan-butanovoj frakcii. A.G. Dedov, A.S. Loktev, L.H. Kunashev, M.N. Kartasheva, V.S. Bogatyrev, I.I. Moiseev. Himicheskaja tehnologija, 2002, no. 8, p. 15–19.
8.
Aktivnye centry ceolita NCVM, promotirovannogo oksidami cinka i hroma. A.G. Dedov, A.S. Loktev, A.N. Harlanov, I.Ju. Kartashev, D.A. Udal’cov, I.I. Moiseev. Zhurnal fizicheskoj himii, 2004. T. 78, no. 11, p. 1980-1985.
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Sposob poluchenija aromaticheskih uglevodorodov (3 varianta). G.V. Echevskij, O.V. Kihtjanin, O.V. Klimov, S.V. Dudarev, A.V. Toktarev, E.G. Kodenev, S.P. Kil’djashev, V.N. Parmon. Patent RF no. 2188225, 2002. Bjul. no. 24.
10. Dergachev A. A., Lapidus A.L. Kataliticheskaja aromatizacija nizshih alkanov. Rossijskij himicheskij zhurnal (Zhurnal Rossijskogo himicheskogo obshhestva im. D.I. Mendeleeva), 2008. T. 52, no. 4, p. 15-21.
11.
Kutepov B.I., Belousova O.Ju. Aromatizacija uglevodorodov na pentasilsoderzhashhih katalizatorah. M.: Himija, 2000, 95 p.
12. Giannetto G., Monque R., Galiasso R. Transformation of LPG into aromatic hydrocarbons and hydrogen over zeolite catalysts. Catalysis Review — Science & Engineering, 1994, vol. 36, no. 2, p. 274-304.
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Templatnyj sintez 3-D strukturirovannyh makroporistyh oksidov i ierarhicheskih ceolitov. E.V. Parhomchuk, K.A. Sashkina, N.A. Rudina, N.A. Kulikovskaja, V.N. Parmon. Kataliz v promyshlennosti, 2012, no. 4, p. 23-32.
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Abello S., Bonilla A., Perez-Ramirez J. Mesoporous ZSM-5 zeolite catalysts prepared by desilication with organic hydroxides and comparison with NaOH leaching. Applied Catalysis A: Gene- ral, 2009, vol. 364, no. 1-2, p. 191-198.
15.
Prjamaja konversija trigliceridov zhirnyh kislot v komponenty motornyh topliv. A.G. Dedov, A.S. Loktev, A.E. Gehman, T.V. Kosakova, E.A. Isaeva, M.N. Kartasheva, I.I. Moiseev. Himicheskaja tehnologija, 2011. T. 12, no. 11, p. 654-662

2009/1
Kinetic parameters of reaction of methane oxidative coupling catalyzed by lantana-ceria oxide system
Oil and gas processing, chemistry of oil and gas

Authors:
Alexey G. DEDOV, corresponding Member of RAS, Doctor of Chemical Science, Professor, Head of Chair of General & Inorganic Chemistry, Gubkin Russian State Oil and Gas University, has ended chemical faculty of the Moscow State University in 1974.
Alexey S. LOKTEV, Doctor of Chemical Science, Assistant Professor, Professor of Chair of General & Inorganic Chemistry, Gubkin Russian State Oil and Gas University, has ended chemical faculty of the Moscow State University in 1974.
Vladilen A. MAKHLIN, PhD, Head of laboratory, Karpov Institute of Physical Chemistry, has ended the Moscow state academy of fine chemical technology in 1960.
Kseniya V. PARHOMENKO, PhD, engineer-researcher of Universite Louis Pasteur, Institut de Chimie, Strasbourg, France, has ended the Gubkin Russian State Oil and Gas University in 2004.
Alexander S. EVENCHIK, PhD, scientific researcher, Karpov Institute of Physical Chemistry, has ended the Moscow institute of chemical mechanical engineering in 1972.
Ilya I. MOISEEV, Academician of RAS, Doctor of Chemical Science, Professor, Professor of Chair of General & Inorganic Chemistry, Gubkin Russian State Oil and Gas University, has ended the Moscow state academy of fine chemical technology in 1952. E-mail: biblioteka@nedrainform.ru

Abstract: Kinetic parameters of dimerization by oxidation of methane on lanthanum-cerium catalyst deposited on MgO (periclase) are identified. Phenomenological description of the obtained kinetic mechanism and numerical values of constants allows to perform engineering calculations so as to choose an optimal design of a commercial reactor.

Index UDK: 542.943.7

Keywords: lanthanum-cerium catalyst, metal dimerization by oxidation

Bibliography: