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

被引:149
作者
Bleken, Francesca [1 ]
Skistad, Wegard [1 ]
Barbera, Katia [2 ]
Kustova, Marina [3 ]
Bordiga, Silvia [2 ]
Beato, Pablo [3 ]
Lillerud, Karl Petter [1 ]
Svelle, Stian [1 ]
Olsbye, Unni [1 ]
机构
[1] Univ Oslo, InGAP Ctr Res Based Innovat, Ctr Mat Sci & Nanotechnol SMN, Dept Chem, N-0315 Oslo, Norway
[2] Univ Turin, Dipartimento Chim, IFM NIS Ctr Excellence, I-10125 Turin, Italy
[3] Haldor Topsoe, DK-2800 Lyngby, Denmark
关键词
TO-HYDROCARBONS REACTION; REACTION-MECHANISM; MTO REACTION; AROMATIC-HYDROCARBONS; CATALYTIC-PROPERTIES; SHAPE SELECTIVITY; LIGHT OLEFINS; MEDIUM-PORE; SAPO-34; TRANSFORMATION;
D O I
10.1039/c0cp01982h
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
Four 3D 10-ring zeolites, IM-5, TNU-9, ZSM-11 and ZSM-5, with Si/Al = 14-24 and crystal sizes below 2 microns, were tested as catalysts for the methanol to hydrocarbons reaction (MTH) at atmospheric pressure, 350 degrees C and WHSV = 9 h (1). All catalysts gave initially full methanol conversion, and showed strikingly similar effluent product selectivities. However, their life-time duration differed significantly, and decreased in the order: ZSM-11 > ZSM-5 >> TNU-9 > IM-5. A main difference between the two groups of stability behaviour was the size of cavities formed by channel intersections; larger cavities in TNU-9 and IM-5 leading to polyaromatics formation and a more rapid deactivation compared to ZSM-5 and ZSM-11. Effluent yield-conversion plots suggested that polymethylated benzene intermediates were more important in IM-5 and TNU-9 than in ZSM-5 and ZSM-11, where alkene methylation and cracking reactions seemed to dominate product formation. However, this difference had only minor influence on effluent selectivity.
引用
收藏
页码:2539 / 2549
页数:11
相关论文
共 51 条
[1]   CATALYTIC CRACKING AND SKELETAL ISOMERIZATION OF NORMAL-HEXENE ON ZSM-5 ZEOLITE [J].
ABBOT, J ;
WOJCIECHOWSKI, BW .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1985, 63 (03) :451-461
[2]   STUDIES ON THE CONVERSION OF ISOPENTANE OVER SHAPE-SELECTIVE ZEOLITES .1. H-ZSM-5 AND H-ZSM-11 ZEOLITES [J].
ANUNZIATA, OA ;
PIERELLA, LB .
REACTION KINETICS AND CATALYSIS LETTERS, 1995, 55 (02) :365-372
[3]   SELECTIVE TRANSFORMATION OF LIGHT OLEFINS INTO AROMATIC-HYDROCARBONS OVER PENTASIL ZEOLITES [J].
ANUNZIATA, OA ;
PIERELLA, LB ;
MARINO, RG .
REACTION KINETICS AND CATALYSIS LETTERS, 1995, 54 (02) :229-237
[4]   TRANSFORMATION OF LIGHT PARAFFINS INTO AROMATIC-HYDROCARBONS OVER H-ZSM-11 ZEOLITE [J].
ANUNZIATA, OA ;
ORIO, OA ;
AGUIRRE, MC ;
PIERELLA, LB .
REACTION KINETICS AND CATALYSIS LETTERS, 1988, 37 (01) :205-210
[5]   The reactivity of molecules trapped within the SAPO-34 cavities in the methanol-to-hydrocarbons reaction [J].
Arstad, B ;
Kolboe, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (33) :8137-8138
[6]   Methanol-to-hydrocarbons reaction over SAPO-34. Molecules confined in the catalyst cavities at short time on stream [J].
Arstad, B ;
Kolboe, S .
CATALYSIS LETTERS, 2001, 71 (3-4) :209-212
[7]   Structure of the polycrystalline zeolite catalyst IM-5 solved by enhanced charge flipping [J].
Baerlocher, Christian ;
Gramm, Fabian ;
Massueger, Lars ;
McCusker, Lynne B. ;
He, Zhanbing ;
Hovmoeller, Sven ;
Zou, Xiaodong .
SCIENCE, 2007, 315 (5815) :1113-1116
[8]  
Baerlocher C, 2007, STUD SURF SCI CATAL, V170, P657
[9]   Persistent methylbenzenium ions in protonated zeolites: The required proton affinity of the guest hydrocarbon [J].
Bjorgen, M ;
Bonino, F ;
Arstad, B ;
Kolboe, S ;
Lillerud, KP ;
Zecchina, A ;
Bordiga, S .
CHEMPHYSCHEM, 2005, 6 (02) :232-235
[10]   Conversion of methanol to hydrocarbons: the reactions of the heptamethylbenzenium cation over zeolite H-beta [J].
Bjorgen, M ;
Olsbye, U ;
Svelle, S ;
Kolboe, S .
CATALYSIS LETTERS, 2004, 93 (1-2) :37-40