Counterion-Controlled Formation of an Octanuclear Uranyl Cage with cis-1,2-Cyclohexanedicarboxylate Ligands

Inorganic Chemistry
Pierre ThuéryJack Harrowfield

Abstract

cis-1,2-Cyclohexanedicarboxylic acid ( c-chdcH2) was reacted with uranyl nitrate under (solvo-)hydrothermal conditions in the presence of different possible counterions. Two neutral complexes of 1:1 stoichiometry were obtained, [UO2( c-chdc)(DMF)] (1) and [UO2( c-chdc)(H2O)] (2), which crystallize as two-dimensional coordination polymers and do not include the additional cations present in solution. In contrast, the complex [NH4][PPh4][(UO2)8( c-chdc)9(H2O)6]·3H2O (3) crystallized in the presence of PPh4Br, ammonium cations being generated in situ from acetonitrile hydrolysis. This complex of 8:9 uranium:ligand stoichiometry contains an octanuclear anionic cage of D3 symmetry with a pseudo-cubic arrangement of uranium atoms. The ammonium cation is held within the cage through four hydrogen bonds with uranyl oxo groups directed inward. This cage complex is luminescent, although with a low quantum yield of 0.06, indicating limited potential as a photo-oxidant of included species.

References

Jun 4, 2004·Journal of the American Chemical Society·Pierre ThuéryBernardo Masci
Apr 19, 2012·Nature Communications·Sara PasqualeJavier de Mendoza
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Dec 2, 2014·Inorganic Chemistry·Jie LingPeter C Burns
Dec 30, 2014·Acta Crystallographica. Section A, Foundations and Advances·George M Sheldrick
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Jan 1, 1997·Methods in Enzymology·Zbyszek Otwinowski, Wladek Minor
Sep 22, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Pierre Thuéry, Jack Harrowfield

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Citations

May 24, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Pierre ThuéryJack Harrowfield

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