期刊
CHEMSUSCHEM
卷 11, 期 21, 页码 3812-3820出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201801486
关键词
heterogeneous catalysis; methanol-to-olefin; SAPO-34; templates; zeolites
资金
- Nation Key Research and Development Program of China [2016YFB0701100]
- National Natural Science Foundation of China [21320102001, 21621001]
- National 111 Project [B17020]
Significant interest has emerged in the development of nanometer-sized and hierarchical silicoaluminophosphate zeolites (SAPO-34) because of their enhanced accessibility and improved catalytic activity for methanol-to-olefin (MTO) conversion. A series of nanometer-sized SAPO-34 catalysts with tunable hierarchical structures was synthesized in a Al2O3/H3PO4/SiO2/triethylamine(TEA)/H2O system by using a mesoporogen-free nanoseed-assisted method. The nanometer-sized hierarchical S-H-3.0 catalyst (TEA/Al2O3=3.0) possessed the highest crystallinity, highest abundance of intracrystalline meso-/macropores, and the most suitable acidity among all obtained catalysts, showing the highest ethylene and propylene selectivity of 85.4 %. This is the highest reported selectivity for MTO reactions under similar conditions. Detailed analysis of the coke produced during the reaction revealed that the small-sized methyl-substituted benzene and bulky methyl-substituted pyrene were mainly located inside the crystals instead of on the surface of the crystals, which provided further insight into understanding the deactivation of the SAPO-34 catalyst during MTO reaction. Significantly, the simple and cost-effective synthetic process and superb catalytic performance of the nanometer-sized hierarchical SAPO-34 is promising for their practical large-scale application for MTO conversion.
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