The Effect of Acid Strength on the Conversion of Methanol to Olefins Over Acidic Microporous Catalysts with the CHA Topology

被引:242
作者
Bleken, Francesca [1 ]
Bjorgen, Morten [2 ]
Palumbo, Luisa [3 ,4 ]
Bordiga, Silvia [3 ,4 ]
Svelle, Stian [1 ]
Lillerud, Karl-Petter [1 ]
Olsbye, Unni [1 ]
机构
[1] Univ Oslo, inGAP Ctr Res Based Innovat, Ctr Mat Sci & Nanotechnol, Dept Chem, N-0315 Oslo, Norway
[2] Norwegian Univ Sci & Technol, Dept Chem, N-7491 Trondheim, Norway
[3] Univ Turin, Dipartimento Chim, IFM, NIS Ctr Excellence, I-10125 Turin, Italy
[4] INSTM Unita Torino Ctr Riferimento, Turin, Italy
基金
欧盟地平线“2020”;
关键词
MTO; H-SAPO-34; H-SSZ-13; CHA; Methanol-to-hydrocarbons; Acid strength; Methanol; Zeolite; Zeotype; TO-HYDROCARBONS REACTION; REACTION-MECHANISM; METHYLATION REACTIONS; PRODUCT SELECTIVITY; REACTION CENTERS; ZEOLITE H-ZSM-5; POOL MECHANISM; MTO REACTION; SAPO-34; CHEMISTRY;
D O I
10.1007/s11244-008-9158-0
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The present work addresses the influence of acid strength on the stability and product selectivity of microporous catalysts with CHA framework type. The two studied catalysts, H-SAPO-34 and H-SSZ-13, have the same topology, density of acid sites (approximately one acid site per cage), and crystal size (0.2-2 microns), but their acid strength differ due to the framework composition. The difference in acid strength was determined by infrared spectroscopy, using CO as probe molecule. Catalytic tests were performed in a fixed bed flow reactor at 300-425 A degrees C and WHSV = 6.0 h(-1). It was observed that the acid strength has significant influence on reaction rates, enhancing the production rate of olefins in the reactor effluent as well as aromatics retained in the catalyst pores and leading to a lower optimal temperature of operation for the more acidic H-SSZ-13 catalyst. The activation and deactivation patterns and the intermediates formed are very similar for the two materials. The ethene to propene ratio increases with temperature and time on stream for both catalysts, and is higher over the more acidic H-SSZ-13 catalyst at similar reaction conditions.
引用
收藏
页码:218 / 228
页数:11
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