Synthesis and characterization of DNL-6, a new silicoaluminophosphate molecular sieve with the RHO framework

被引:32
作者
Su, Xiong [1 ,2 ,3 ]
Tian, Peng [1 ,2 ]
Li, Jinzhe [1 ,2 ]
Zhang, Ying [1 ,2 ]
Meng, Shuanghe [1 ,2 ]
He, Yanli [1 ,2 ]
Fan, Dong [1 ,2 ,3 ]
Liu, Zhongmin [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China
[3] Chinese Acad Sci, Grad Univ, Beijing 100049, Peoples R China
关键词
SAPO; RHO; Synthesis; DNL-6; Crystallization mechanism; SOLID-STATE NMR; ZEOLITE RHO; CRYSTAL-STRUCTURES; ALUMINOPHOSPHATE; CRYSTALLIZATION; CATION;
D O I
10.1016/j.micromeso.2011.04.004
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A new silicoaluminophosphate molecular sieve with the RHO framework (designated as DNL-6, Dalian National Laboratory Number 6) has been hydrothermally synthesized for the first time with diethylamine (DEA) template in the presence of cetyltrimethylammonium bromide (CTAB). Influence factors, such as CTAB amount and silica content in the starting gel, crystallization time and temperature, were investigated. It was observed that DEA together with CTAB were necessary for the formation of pure RHO phase, which appeared in a narrow range of the starting gel compositions and synthesis conditions. Only DEA and water molecules were found in the as-synthesized DNL-6 without any existence of CTAB. All Si atoms incorporated into the framework with Si(4Al) environment at a high amount close to the theoretical maximum value. DNL-6 molecular sieve possessed high micropore surface area (777 m(2)/g) and large micropore volume (0.36 cm(3)/g) with good thermal and hydrothermal stability. Crystallization course was studied by monitoring solid products at different crystallization times with XRD, SEM, XRF, NMR and CHN elemental analysis. It is proposed that DNL-6 crystals were more likely formed directly from the crystallization of liquid phase rather than from the transformation of amorphous materials, and Si atoms directly incorporated into the DNL-6 framework from the very beginning of the crystallization via a SM2 mechanism. (C) 2011 Elsevier Inc. All rights reserved.
引用
收藏
页码:113 / 119
页数:7
相关论文
共 34 条
[1]  
Baerlocher Ch., Database of zeolite structures
[2]   Rigid unit modes and the phase transition and structural distortions of zeolite rho [J].
Bieniok, A ;
Hammonds, KD .
MICROPOROUS AND MESOPOROUS MATERIALS, 1998, 25 (1-3) :193-200
[3]   SOLID-STATE NMR OF SILICOALUMINOPHOSPHATE MOLECULAR-SIEVES AND ALUMINOPHOSPHATE MATERIALS [J].
BLACKWELL, CS ;
PATTON, RL .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (13) :3965-3970
[4]  
Breck D W, 1985, The United States, Patent No. [US4503023, 4503023]
[5]   Successive steps of hydration and dehydration of silicoaluminophosphates H-SAPO-34 and H-SAPO-37 investigated by in situ CF MAS NMR spectroscopy [J].
Buchholz, A ;
Wang, W ;
Arnold, A ;
Xu, M ;
Hunger, M .
MICROPOROUS AND MESOPOROUS MATERIALS, 2003, 57 (02) :157-168
[6]   Co-templating and modelling in the rational synthesis of zeolitic solids [J].
Castro, Maria ;
Garcia, Raquel ;
Warrender, Stewart J. ;
Slawin, Alexandra M. Z. ;
Wright, Paul A. ;
Cox, Paul A. ;
Fecant, Antoine ;
Mellot-Draznieks, Caroline ;
Bats, Nicolas .
CHEMICAL COMMUNICATIONS, 2007, (33) :3470-3472
[7]   Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts [J].
Choi, Minkee ;
Na, Kyungsu ;
Kim, Jeongnam ;
Sakamoto, Yasuhiro ;
Terasaki, Osamu ;
Ryoo, Ryong .
NATURE, 2009, 461 (7261) :246-U120
[8]   FLEXIBILITY OF THE ZEOLITE RHO FRAMEWORK - INSITU X-RAY AND NEUTRON POWDER STRUCTURAL CHARACTERIZATION OF DIVALENT CATION-EXCHANGED ZEOLITE RHO [J].
CORBIN, DR ;
ABRAMS, L ;
JONES, GA ;
EDDY, MM ;
HARRISON, WTA ;
STUCKY, GD ;
COX, DE .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1990, 112 (12) :4821-4830
[9]   INORGANIC SOLID ACIDS AND THEIR USE IN ACID-CATALYZED HYDROCARBON REACTIONS [J].
CORMA, A .
CHEMICAL REVIEWS, 1995, 95 (03) :559-614
[10]   Ordered porous materials for emerging applications [J].
Davis, ME .
NATURE, 2002, 417 (6891) :813-821