Synthesis of 10 and 12 Ring Zeolites (MCM-22, TNU-9 and MCM-68) Modified with Zn and Its Potential Application in the Reaction of Methanol to Light Aromatics and Olefins

被引：12

作者：

Garcia-Ruiz, Misael ^{[1
]}

Solis-Casados, Dora A. ^{[2
]}

Aguilar-Pliego, Julia ^{[3
]}

Marquez-Alvarez, Carlos ^{[4
]}

Sastre-de Andres, Enrique ^{[4
]}

Sanjurjo-Tartalo, Diana ^{[4
]}

Sainz-Vaque, Raquel ^{[4
]}

Grande-Casas, Marisol ^{[4
]}

机构：

[1] Univ Autonoma Estado Mexico, Ciencia Mat, Fac Quim, Paseo Colon Esquina Paseo Tollocan S-N, Toluca 50000, Estado De Mexic, Mexico

[2] Univ Autonoma Estado Mexico, Ctr Conjunto Invest Quim Sustentable, UNAM, Personal Acad Adscrito,Fac Quim, Toluca, Estado De Mexic, Mexico

[3] UAM A, Area Quim Aplicada, Dept Ciencias Basicas, San Pablo 180, Cuidad De Mexico 02200, Mexico

[4] CSIC, Inst Catalisis & Petroleoquim, C Marie Curie 2,Campus Cantoblanco, Madrid 28049, Spain

来源：

TOPICS IN CATALYSIS | 2020年 / 63卷 / 5-6期

关键词：

Methanol conversion; Aromatics compounds; BTX fraction; Zeolites modified; Light olefins; CATALYTIC PERFORMANCE; PARTICLE-SIZE; CONVERSION; ZSM-5; ACIDITY; AROMATIZATION; ISOMERIZATION; HYDROCARBONS; ALKYLATION; MORPHOLOGY;

D O I：

10.1007/s11244-020-01242-x

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The effect on the incorporation of zinc of three zeolites TNU-9, MCM-22, and MCM-68 was investigated. The physico-chemical properties of zeolites were studied by X-ray diffraction, N-2-adsorption, temperature-programmed desorption of NH3 (TPD), nuclear magnetic resonance of Al-27 and Si-29 (MAS NMR), scanning electron microscopy (SEM) and thermogravimetric analysis (TGA). Then all the samples were characterized and evaluated in the reaction of methanol to aromatics (MTA). The correlation of zinc incorporation method and acidic properties of zeolites with catalytic performance was investigated. The form of zinc incorporation, the acidity, the type of zeolitic structure and the reaction temperature had a great influence on the catalytic activity. Regarding the type of structure, the total aromatics selectivity in this work increased in the followed order for zeolites modified with Zn: MCM-68 > TNU-15 > MCM-22. The medium pore zeolite T9-15 (TNU-9 zeolite and Si/Al 15 ratio) catalysts with the ratio ZnO/ZnO + Al2O3 equal to 0.34 (T9-15 0.5 Zn) showed better stability with conversion of methanol completes during 9 h of reaction and 17% to BTX selectivity and 32% to total aromatics compounds at 450 degrees C and WHSV of 4.24 h(-1). In methanol conversion, the selectivity to aromatics over the T9-15 modified-Zn materials (TNU-9 zeolite and Si/Al 15 ratio) under study, increased in the followed order: T9-15 0.5 Zn > ZT9-15 > T9-15 > T9-15 0.2 Zn. The reaction temperature is an important variable in the MTA process. At 450 degrees C a better activation of acid sites is achieved in zeolite with Zn and therefore a high percentage of BTX selectivity is obtained for TNU-9 zeolite.

引用

页码：451 / 467

页数：17

共 54 条

[1] Recent Advances in Reactions of Alkylbenzenes Over Novel Zeolites: The Effects of Zeolite Structure and Morphology [J].

Al-Khattaf, Sulaiman ;

Ali, Syed A. ;

Aitani, Abdullah M. ;

Zilkova, Nadezda ;

Kubicka, David ;

Cejka, Jiri .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2014, 56 (04) :333-402

[2] Catalytic pyrolysis of central German lignite in a semi-continuous rotary kiln - Performance of pulverized one-way ZSM-5 catalyst and ZSM-5-coated beads [J].

Appelt, J. ;

Heschel, W. ;

Meyer, B. .

FUEL PROCESSING TECHNOLOGY, 2016, 144 :56-63

[3] Biomass to liquid transportation fuels (BTL) systems: process synthesis and global optimization framework [J].

Baliban, Richard C. ;

Elia, Josephine A. ;

Floudas, Christodoulos A. .

ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (01) :267-287

[4] Methanol to gasoline over zeolite H-ZSM-5: Improved catalyst performance by treatment with NaOH [J].

Bjorgen, Morten ;

Joensen, Finn ;

Holm, Martin Spangsberg ;

Olsbye, Unni ;

Lillerud, Karl-Petter ;

Svelle, Stian .

APPLIED CATALYSIS A-GENERAL, 2008, 345 (01) :43-50

[5] Conversion of methanol over 10-ring zeolites with differing volumes at channel intersections: comparison of TNU-9, IM-5, ZSM-11 and ZSM-5 [J].

Bleken, Francesca ;

Skistad, Wegard ;

Barbera, Katia ;

Kustova, Marina ;

Bordiga, Silvia ;

Beato, Pablo ;

Lillerud, Karl Petter ;

Svelle, Stian ;

Olsbye, Unni .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (07) :2539-2549

[6] Isomerization and hydrocracking of heptane over bimetallic bifunctional PtPd/H-beta and PtPd/USY zeolite catalysts [J].

Blomsma, E ;

Martens, JA ;

Jacobs, PA .

JOURNAL OF CATALYSIS, 1997, 165 (02) :241-248

[7]

Calabro D.C., 2000, Patent No. [6,049018, 6049018, US6049018A]

[8] SYNTHESIS AND CHARACTERIZATION OF THE MCM-22 ZEOLITE [J].

CORMA, A ;

CORELL, C ;

PEREZPARIENTE, J .

ZEOLITES, 1995, 15 (01) :2-8

[9] Synthesis of MCM-22 zeolites of different Si/Al ratio and their structural, morphological and textural characterisation [J].

Delitala, C. ;

Alba, M. D. ;

Becerro, A. I. ;

Delpiano, D. ;

Meloni, D. ;

Musu, E. ;

Ferino, I. .

MICROPOROUS AND MESOPOROUS MATERIALS, 2009, 118 (1-3) :1-10

[10] Crystal structure of zeolite MCM-68: A new three-dimensional framework with large pores [J].

Dorset, DL ;

Weston, SC ;

Dhingra, SS .

JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (05) :2045-2050

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