Location of the fluoride ion in tetrapropylammonium fluoride silicalite-1 determined by 1H/19F/29Si triple resonance CP, REDOR, and TEDOR NMR experiments

被引:131
作者
Fyfe, CA
Brouwer, DH
Lewis, AR
Chézeau, JM
机构
[1] Univ British Columbia, Dept Chem, Vancouver, BC V6T 1Z1, Canada
[2] Ecole Natl Super Chim, UPRES A 7016 CNRS, Lab Mat Mineraux, F-68093 Mulhouse, France
基金
中国国家自然科学基金;
关键词
D O I
10.1021/ja010532v
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The location of the fluoride ion in tetrapropylammonium fluoride silicalite-1 ([TPA]-F-[Si-MFI]), an as-synthesized siliceous zeolite with the MEI topology, has been unambiguously determined using solid-state NMR experiments alone. With the H-1 --> Si-29 CP-INADEQUATE experiment, the 12 peaks in the highly resolved Si-29 MAS NMR spectrum of [TPA]-F-[Si-MFI] were assigned. Using these peak assignments it was possible to perform H-1/F-19/Si-29 triple resonance CP, REDOR, and TEDOR experiments to measure F-Si distances and thus locate the fluoride ion. It is covalently bonded to Si-9 in the [4(1)5(2)6(2)] cage of the zeolite framework and exchanges between two "mirror-related" Si-9 sites, making them equivalent on the NMR time scale. The importance of this result and the general applicability of the approach are discussed.
引用
收藏
页码:6882 / 6891
页数:10
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