SAPO-34 templated by dipropylamine and diisopropylamine: synthesis and catalytic performance in the methanol to olefin (MTO) reaction

被引:32
作者
Fan, Dong [1 ,2 ]
Tian, Peng [1 ]
Xu, Shutao [1 ]
Wang, Dehua [1 ,2 ]
Yang, Yue [1 ]
Li, Jinzhe [1 ]
Wang, Quanyi [1 ]
Yang, Miao [1 ]
Liu, Zhongmin [1 ,3 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
CRYSTALLINE INORGANIC SOLIDS; STRUCTURE-DIRECTING AGENTS; MOLECULAR-SIEVES; MICROPOROUS MATERIALS; PRODUCT SELECTIVITY; SI DISTRIBUTION; RATIONAL SYNTHESIS; REACTION CENTERS; CONVERSION; FRAMEWORK;
D O I
10.1039/c5nj02351c
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In this work, a comprehensive study of the hydrothermal synthesis and catalytic performance of SAPO-34 templated by the isomeric dipropylamine (DPA) and diisopropylamine (DIPA) was carried out. SAPO-34 with a faster crystallization rate and lower Si content could be obtained with DIPA as the template, suggesting the better templating efficacy of DIPA than DPA. Theoretical calculations reveal that DIPA possesses more favourable non-bonding interactions with the CHA framework and the electronic configuration is of vital importance in determining the template efficacy. SAPO-34-DIPA with low silicon contents exhibits excellent performance, over which a maximum selectivity of ethylene plus propylene (87.2%) is observed. This value should be among the top ever reported. The surface Si enrichment on the crystals, which is both template- and condition-dependent, is revealed to be of significant influence in the catalytic performance. The relatively homogenous Si distribution in the crystals, lower acid concentration and weaker acid strength corporately make SAPO-34-DIPA an excellent MTO catalyst.
引用
收藏
页码:4236 / 4244
页数:9
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