Molecular engineering of microporous crystals: (IV) Crystallization process of microporous aluminophosphate AlPO4-11

被引:27
作者
Cheng, Tao [2 ]
Xu, Jun [3 ]
Li, Xu [1 ]
Li, Yi [1 ]
Zhang, Bin [1 ]
Yan, Wenfu [1 ]
Yu, Jihong [1 ]
Sun, Huai [2 ]
Deng, Feng [3 ]
Xu, Ruren [1 ]
机构
[1] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China
[2] Shanghai Jiao Tong Univ, Coll Chem & Chem Engn, Shanghai 200240, Peoples R China
[3] Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Wuhan 430071, Peoples R China
基金
中国国家自然科学基金;
关键词
Aluminophosphate; AlPO4-11; Fragment; Crystallization; Zeolite; MFI ZEOLITE; SILICALITE-1; CRYSTALLIZATION; STRUCTURE DIRECTION; ZEOSIL NANOSLABS; UV-RAMAN; MECHANISM; TPAOH-TEOS-H2O; SIEVE; IDENTIFICATION; PHOSPHATES;
D O I
10.1016/j.micromeso.2011.11.034
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The products of microporous aluminophosphate AlPO4-11 crystallized for different periods of time were freeze-dried and characterized by XRD and NMR techniques. Six crystallographically distinct Al- and P-centered large fragments and 34 small fragments of dimer (Al-P), trimer (Al-P-Al and P-Al-P), tetramer (Al-P-3 and P-Al-3). pentamer (Al-P-4 and P-Al-4), and 4- and 6-membered rings were extracted from the framework of AlPO4-11. Each of the six large fragments contained two completed coordination layers surrounding the centered atom. The shielding tensors of the Al and P atoms of the fragments were calculated using the quantum mechanics density functional theory. The experimentally observed chemical shifts of Al or P from the well-crystallized AlPO4-11 were assigned to the shielding tensors of the center atoms of the six large fragments and were further used as references in the determination of the chemical shifts of the Al or P atoms in the small fragments. A comparison of the calculated chemical shifts of the Al and P atoms in the small fragments to the experimental data of the products isolated at different crystallization periods suggested that the fragments of dimers, trimers of the form Al-P-Al, tetramers of the form P-Al-3, and pentamers may exist in the crystallization process of AlPO4-11. On the basis of these observations regarding the putative small fragments, a possible crystallization process of AlPO4-11 was proposed. (C) 2011 Elsevier Inc. All rights reserved.
引用
收藏
页码:190 / 207
页数:18
相关论文
共 71 条
[1]   Methods for in situ spectroscopic probing of the synthesis of a zeolite [J].
Aerts, Alexander ;
Kirschhock, Christine E. A. ;
Martens, Johan A. .
CHEMICAL SOCIETY REVIEWS, 2010, 39 (12) :4626-4642
[2]   Investigation of the Mechanism of Colloidal Silicalite-1 Crystallization by Using DLS, SAXS, and 29Si NMR Spectroscopy [J].
Aerts, Alexander ;
Haouas, Mohamed ;
Caremans, Tom P. ;
Follens, Lana R. A. ;
van Erp, Titus S. ;
Taulelle, Francis ;
Vermant, Jan ;
Martens, Johan A. ;
Kirschhock, Christine E. A. .
CHEMISTRY-A EUROPEAN JOURNAL, 2010, 16 (09) :2764-2774
[3]  
[Anonymous], 2005, MAT STUD V4 0
[4]   STRUCTURES OF ETHYLENEDIAMMONIUM MONOHYDROGENTETRAOXOPHOSPHATE(V) AND ETHYLENEDIAMMONIUM MONOHYDROGENTETRAOXOARSENATE(V) [J].
AVERBUCHPOUCHOT, MT ;
DURIF, A .
ACTA CRYSTALLOGRAPHICA SECTION C-CRYSTAL STRUCTURE COMMUNICATIONS, 1987, 43 :1894-1896
[5]  
Baerlocher Ch., Database of zeolite structures
[6]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[7]   ALUMINOPHOSPHATE MOLECULAR-SIEVE AIPO4-11 - PARTIAL REFINEMENT FROM POWDER DATA USING A PULSED NEUTRON SOURCE [J].
BENNETT, JM ;
RICHARDSON, JW ;
PLUTH, JJ ;
SMITH, JV .
ZEOLITES, 1987, 7 (02) :160-162
[8]  
Breck DW., 1974, Zeolite Molecular Sieves
[9]   MECHANISM OF STRUCTURE DIRECTION IN THE SYNTHESIS OF SI-ZSM-5 - AN INVESTIGATION BY INTERMOLECULAR H-1-SI-29 CP MAS NMR [J].
BURKETT, SL ;
DAVIS, ME .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (17) :4647-4653
[10]   MECHANISMS OF STRUCTURE DIRECTION IN THE SYNTHESIS OF PURE-SILICA ZEOLITES .1. SYNTHESIS OF TPA/SI-ZSM-5 [J].
BURKETT, SL ;
DAVIS, ME .
CHEMISTRY OF MATERIALS, 1995, 7 (05) :920-928