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
相关论文
共 51 条
  • [1] Baerlocher Ch., Database of zeolite structures
  • [2] INFLUENCE OF THE CHOICE OF THE TEMPLATE ON THE SHORT-TERM AND LONG-TERM STABILITY OF SAPO-34 ZEOLITE
    BRIEND, M
    VOMSCHEID, R
    PELTRE, MJ
    MAN, PP
    BARTHOMEUF, D
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (20) : 8270 - 8276
  • [3] SSZ-53 and SSZ-59: Two novel extra-large pore zeolites
    Burton, A
    Elomari, S
    Chen, CY
    Medrud, RC
    Chan, IY
    Bull, LM
    Kibby, C
    Harris, TV
    Zones, SI
    Vittoratos, ES
    [J]. CHEMISTRY-A EUROPEAN JOURNAL, 2003, 9 (23) : 5737 - 5748
  • [4] Ordered porous materials for emerging applications
    Davis, ME
    [J]. NATURE, 2002, 417 (6891) : 813 - 821
  • [5] Synthesis, characterization and catalytic activity of SAPO-34 obtained with piperidine as templating agent
    Dumitriu, E
    Azzouz, A
    Hulea, V
    Lutic, D
    Kessler, H
    [J]. MICROPOROUS MATERIALS, 1997, 10 (1-3): : 1 - 12
  • [6] Strong templating effect of TEAOH in the hydrothermal genesis of the AlPO4-5 molecular sieve:: Experimental and computational investigations
    Elanany, Mohamed
    Su, Bao-Lian
    Vercauteren, Daniel P.
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2007, 270 (1-2) : 295 - 301
  • [7] Aminothermal synthesis of CHA-type SAPO molecular sieves and their catalytic performance in methanol to olefins (MTO) reaction
    Fan, Dong
    Tian, Peng
    Su, Xiong
    Yuan, Yangyang
    Wang, Dehua
    Wang, Chan
    Yang, Miao
    Wang, Linying
    Xu, Shutao
    Liu, Zhongmin
    [J]. JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (45) : 14206 - 14213
  • [8] A novel solvothermal approach to synthesize SAPO molecular sieves using organic amines as the solvent and template
    Fan, Dong
    Tian, Peng
    Xu, Shutao
    Xia, Qinghua
    Su, Xiong
    Zhang, Lin
    Zhang, Ying
    He, Yanli
    Liu, Zhongmin
    [J]. JOURNAL OF MATERIALS CHEMISTRY, 2012, 22 (14) : 6568 - 6574
  • [9] Supramolecular chemistry in the structure direction of microporous materials from aromatic structure-directing agents
    Gomez-Hortigueela, Luis
    Lopez-Arbeloa, Fernando
    Cora, Furio
    Perez-Pariente, Joaquin
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (40) : 13274 - 13284
  • [10] Molecular Insights into the Self-Aggregation of Aromatic Molecules in the Synthesis of Nanoporous Aluminophosphates: A Multilevel Approach
    Gomez-Hortigueela, Luis
    Hamad, Said
    Lopez-Arbeloa, Fernando
    Pinar, Ana B.
    Perez-Pariente, Joaquin
    Cora, Furio
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (45) : 16509 - 16524