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Title: Circularly polarized luminescence/total luminescence and conductometric studies of lanthanide-chiral crown ether complexes in solution

Thesis/Dissertation ·
OSTI ID:6908821

The focus of this research was to elucidate the structure and stoichiometry of europium (III) and terbium (III) complexes of chiral 15-crown-5 and 18-crown-6 macrocycles dissolved in the solvents acetonitrile (MeCN), 2,2,2-trifluoroethanol (TFE), and 1,1,1,3,3,3-hexafluoroisopropanol (HFiP). The chiral 15-crown-5 ethers synthesized in this work are (2R,3R)-2,3-dimethyl-1,4,7,10,13-pentaoxacyclopentadecane (2,3-15c5) and its isomer (2S,6S)-2,6-dimethyl-1,4,7,10,13-pentaoxacyclopentadecane (2,6-15c5). The chiral 18-crown-6 ligands employed in this study are (2R,3R)-2,3-dimethyl-1,4,7,10,13,16-hexaoxacyclooctadecane (2,3-18c6), (2S,6S)-2,6-dimethyl-1,4,7,10,13,16-hexaoxacyclooctadecane (2,6-18c6), (2R,3R,11R,12R)-2,3,11,12-tetramethyl-1,4,7,10,13,16-hexaoxacyclooctadecane (2,3,11,12-18c6), and (2S,6S,11S,15S)-2,6,11,15-tetramethyl-1,4,7,10,13-16-hexaoxacyclooctadecane (2,6,11,15-18c6). As probes of the crown-lanthanide association, the techniques of circularly polarized luminescence (CPL) and total luminescence (TL), were employed. Changes in CPL/TL spectra and the simultaneously measured conductivity observed during a titration of Eu(NO/sub 3/)/sub 3/ dissolved in TFE with 2,6-15c5 indicate that the crown-lanthanide nitrate complex is of 1:1 stoichiometry. Complexes between the dimethyl 15-crown-5 ligands and Eu-(ClO/sub 4/)/sub 3/ and Tb(ClO/sub 4/)/sub 3/ adopt a structure similar to that of the nitrate compounds. In TFE, changes in the CPL/TL and conductivity observed during titrations of Eu(ClO/sub 4/)/sub 3/ and Tb(ClO/sub 4/)/sub 3/ with 2,6-15c5 support the formation of 1:2 (lanthanide:crown) sandwich compounds in the presence of an excess of the polyether.

Research Organization:
Duke Univ., Durham, NC (USA)
OSTI ID:
6908821
Resource Relation:
Other Information: Thesis (Ph. D.)
Country of Publication:
United States
Language:
English