Observation and reactivity of the chainlike species ([Al(PO4)2]3-)n during the X-ray diffraction investigation of the hydrothermal synthesis of the super-sodalite sodium aluminophosphate MIL-74 (Na2Al7(PO4)12•4trenH3•Na(H2O)16)

被引:40
作者
Loiseau, T
Beitone, L
Millange, F
Taulelle, F
O'Hare, D
Férey, G
机构
[1] Univ Versailles, CNRS, UMR 8637, Inst Lavoisier, F-78035 Versailles, France
[2] Univ Oxford, Inorgan Chem Lab, Oxford OX1 3QR, England
关键词
D O I
10.1021/jp0485901
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The hydrothermal synthesis of the aluminum phosphate Na2Al7(PO4)(12).4trenH(3).Na(H2O)(16) (MIL-74) has been studied by X-ray diffraction (conventional source) and in-situ time-resolved energy-dispersive X-ray diffraction (synchrotron radiation). Before the crystallization of MIL-74, the reaction of the starting aqueous aluminophosphate gel containing the tren species (tris(2-aminoethyl)amine) and sodium hydroxide gives rise to the formation of a hydrated chainlike solid Al(PO4)(2).trenH(3).6H(2)O (phase 1), which transforms into the hydrate Al(PO4)(2).trenH(3).2.5H(2)O (phase 2) upon heating at 180 degreesC. Its structure was determined by means of single-crystal X-ray diffraction and consists of a one-dimensional inorganic chain of tetrahedral unit AlO4 alternating with the phosphate group PO4. The resulting ([Al(PO4)(2)](3-))(n) chains interact through hydrogen bonds with the trenH(3) and water molecules, generating a layerlike inorganic-organic network. Phase 2 was observed to be an intermediate, which disappears when the MIL-74 solid starts to crystallize. The observation of such an intermediate phase allows for the proposition of a chemical reaction pathway for the formation of the three-dimensional network of MIL-74. It seems that the sodium cations play a crucial role and directly react with the chainlike precursor. They would participate in the construction of the inorganic framework as anchorage nodes during the condensation process.
引用
收藏
页码:20020 / 20029
页数:10
相关论文
共 53 条
[1]   Role of chains in the formation of extended framework tin(II) phosphates and related materials [J].
Adair, BA ;
Neeraj, S ;
Cheetham, AK .
CHEMISTRY OF MATERIALS, 2003, 15 (07) :1518-1529
[2]   Linear-chain AlPOs obtained by the reaction of amine phosphates with Al3+ ions [J].
Ayi, AA ;
Choudhury, A ;
Natarajan, S .
JOURNAL OF SOLID STATE CHEMISTRY, 2001, 156 (01) :185-193
[3]   Tetrahedrally coordinated iron(II) incorporation in the super-sodalite aluminophosphate Fe3Al6(PO4)12•4tren•17H2O (MIL-74) [J].
Beitone, L ;
Loiseau, T ;
Millange, F ;
Huguenard, C ;
Fink, G ;
Taulelle, F ;
Grenèche, JM ;
Férey, G .
CHEMISTRY OF MATERIALS, 2003, 15 (24) :4590-4597
[4]   Order-disorder in the super-sodalite Zn3Al6(PO4)12, 4tren, 17H2O (MIL-74):: A combined XRD-NMR assessment [J].
Beitone, L ;
Huguenard, C ;
Gansmüller, A ;
Henry, M ;
Taulelle, F ;
Loiseau, T ;
Férey, G .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (30) :9102-9110
[5]  
BEITONE L, UNPUB
[6]   In situ studies of the sol-gel synthesis of materials [J].
Cheetham, AK ;
Mellot, CF .
CHEMISTRY OF MATERIALS, 1997, 9 (11) :2269-2279
[7]  
Cheetham AK, 1999, ANGEW CHEM INT EDIT, V38, P3268, DOI 10.1002/(SICI)1521-3773(19991115)38:22<3268::AID-ANIE3268>3.0.CO
[8]  
2-U
[9]   In situ synchrotron x-ray powder diffraction studies of crystallization of microporous aluminophosphates and Me2+-substituted aluminophosphates [J].
Christensen, AN ;
Jensen, TR ;
Norby, P ;
Hanson, JC .
CHEMISTRY OF MATERIALS, 1998, 10 (06) :1688-1693
[10]   Following the crystallization of microporous solids using EDXRD techniques [J].
Davies, AT ;
Sankar, G ;
Catlow, CRA ;
Clark, SM .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (48) :10115-10120