Catalytic conversion of natural gas with added ethane and LPG over Zn-ZSM-11

被引:49
作者
Anunziata, OA [1 ]
Eimer, GA [1 ]
Pierella, LB [1 ]
机构
[1] Univ Tecnol Nacl, Fac Cordoba, Ctr Invest & Tecnol Quim, CITeQ, RA-5016 Cordoba, Argentina
关键词
natural gas conversion; methane activation; aromatic hydrocarbons; MEL zeolites; zinc containing zeolites;
D O I
10.1016/S0926-860X(99)00297-5
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
The higher hydrocarbons (C2+) from natural gas (NG), such as ethane (C2), propane (C3) and butane (C4) reached excellent levels of conversion over Zn-ZSM-11 at temperatures between 550-640 degrees C and 1 atm total pressure, but the methane (C1) present in NG could not be converted. The C1 transformation by activation with co-reactants such as C2 and liquefied petroleum gas (LPG), over Zn-ZSM-11 was studied. The addition of amounts of C2 to a feed of commercial NG allowed to activate the C1 reaching excellent values of conversion and yield to aromatic hydrocarbons (AH). The high Lewis/Bronsted sites ratio of Zn-ZSM-11 catalyst determined by pyridine desorption at different temperatures followed by FT-IR spectroscopy, allowed us to suggest that electron-donor-acceptor complex, formed between C2+ species and unoccupied molecular orbital of the zinc species present in the catalyst, favored the interaction of C2+ through carbenium intermediate to activate methane. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:169 / 176
页数:8
相关论文
共 25 条
[1]   AROMATIZATION OF NATURAL PROPANE USING MODIFIED MOLECULAR-SHAPE SELECTIVE ZEOLITES [J].
ANUNZIATA, OA ;
PIERELLA, LB ;
ORIO, OA .
REACTION KINETICS AND CATALYSIS LETTERS, 1991, 43 (01) :67-73
[2]   ZN-ZSM-11 ZEOLITE CATALYST FOR LPG AROMATIZATION [J].
ANUNZIATA, OA ;
PIERELLA, LB .
CATALYSIS LETTERS, 1992, 16 (04) :437-441
[3]   Methane transformation into aromatic hydrocarbons by activation with LPG over Zn-ZSM-11 zeolite [J].
Anunziata, OA ;
Eimer, GA ;
Pierella, LB .
CATALYSIS LETTERS, 1999, 58 (04) :235-239
[4]   NORMAL-PENTANE CONVERSION TO AROMATIC-HYDROCARBONS OVER ZN-ZSM-11 ZEOLITE [J].
ANUNZIATA, OA ;
ORIO, OA ;
PIERELLA, LB ;
AGUIRRE, MC .
REACTION KINETICS AND CATALYSIS LETTERS, 1989, 39 (01) :75-80
[5]   Direct aromatization of natural gas over H-gallosilicate (MFI), H-galloaluminosilicate (MFI) and Ga/H-ZSM-5 zeolites [J].
Choudhary, VR ;
Kinage, AK ;
Choudhary, TV .
APPLIED CATALYSIS A-GENERAL, 1997, 162 (1-2) :239-248
[6]  
Colitti M, 1998, STUD SURF SCI CATAL, V119, P1
[7]   DETERMINATION OF INTEGRATED MOLAR EXTINCTION COEFFICIENTS FOR INFRARED-ABSORPTION BANDS OF PYRIDINE ADSORBED ON SOLID ACID CATALYSTS [J].
EMEIS, CA .
JOURNAL OF CATALYSIS, 1993, 141 (02) :347-354
[8]   TRANSFORMATION OF LPG INTO AROMATIC-HYDROCARBONS AND HYDROGEN OVER ZEOLITE CATALYSTS [J].
GIANNETTO, G ;
MONQUE, R ;
GALIASSO, R .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1994, 36 (02) :271-304
[9]   CONVERSION OF LIGHT ALKANES TO AROMATIC-HYDROCARBONS .2. ROLE OF GALLIUM SPECIES IN PROPANE TRANSFORMATION ON GAHZSM5 CATALYSTS [J].
GNEP, NS ;
DOYEMET, JY ;
SECO, AM ;
RIBEIRO, FR ;
GUISNET, M .
APPLIED CATALYSIS, 1988, 43 (01) :155-166
[10]  
GNEP NS, 1987, APPL CATAL, V35, P12