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Interaction of Cesium Ions with Calix[4]arene-bis(t-octylbenzo-18-crown-6): NMR and Theoretical Study

Journal Article · · Journal of Physical Chemistry B
DOI:https://doi.org/10.1021/jp203221k· OSTI ID:1017337
 [1];  [2];  [3];  [4]
  1. Institute of Macromolecular Chemistry, Prague
  2. University of West Bohemia, Pilsen, Czech Republic
  3. Institute of Chemical Technology, Prague, Czech Republic
  4. ORNL

Using 1H, 13C, and 133Cs NMR spectra, it is shown that calix[4]arene-bis (t-octylbenzo-18-crown-6) (L) forms complexes with one (L 3 Cs ) and two (L 3 2Cs ) Cs ions offered by cesium bis(1,2-dicarbollide) cobaltate (CsDCC) in nitrobenzene-d5. The ions interact with all six oxygen atoms in the crown-ether ring and the electrons of the calixarene aromatic moieties. According to extraction technique, the stability constant of the first complex is log nb(L 3 Cs ) = 8.8 ( 0.1. According to 133Cs NMR spectra, the value of the equilibrium constant of the second complex is log Knb (2)(L 3 2Cs ) = 6.3(0.2, i.e., its stabilization constant is log nb(L 3 2Cs ) = 15.1 ( 0.3. Self-diffusion measurements by 1H pulsed-field gradient (PFG) NMRcombined with density functional theory (DFT) calculations suggest that one DCC ion is tightly associated with L 3 Cs , decreasing its positive charge and consequently stabilizing the second complex, L 3 2Cs . Using a saturation-transfer 133Cs NMR technique, the correlation times ex of chemical exchange between L 3 Cs and L 3 2Cs as well as between L 3 2Cs and free Cs ions were determined as 33.6 and 29.2 ms, respectively.

Research Organization:
Oak Ridge National Laboratory (ORNL)
Sponsoring Organization:
SC USDOE - Office of Science (SC)
DOE Contract Number:
AC05-00OR22725
OSTI ID:
1017337
Journal Information:
Journal of Physical Chemistry B, Journal Name: Journal of Physical Chemistry B Journal Issue: 23 Vol. 115; ISSN 1520-6106
Country of Publication:
United States
Language:
English