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Closed Uranyl-Dicarboxylate Oligomers: A Tetranuclear Metallatricycle With Uranyl Bridgeheads and 1,3-Adamantanediacetate Linkers

Closed Uranyl-Dicarboxylate Oligomers: A Tetranuclear Metallatricycle With Uranyl Bridgeheads and 1,3-Adamantanediacetate Linkers

Pierre Thuéry, Youssef Atoini, Jack Harrowfield

Inorg Chem. 2018 Jul 2;57(13):7932-7939.

PMID: 29889513

Abstract:

In the presence of NH4+ and either PPh4+ or PPh3Me+ cations, 1,3-adamantanediacetic acid (H2ADA) reacts with uranyl ions under solvo-hydrothermal conditions to give the complexes [NH4]2[PPh4]2[(UO2)4(ADA)6] (1) and [NH4]2[PPh3Me]2[(UO2)4(ADA)6] (2), both of which contain a tetranuclear metallatricycle built from two 2:2 rings including convergent ligands, linked by two additional ligands in an extended conformation defining a third, larger ring. While the ammonium cations are closely associated with the 2:2 rings through triple hydrogen bonding, the large PPh4+ or PPh3Me+ cations are more loosely bound to each of the two faces of the larger ring. In contrast, the complex [H2NMe2][PPh3Me][(UO2)2(ADA)3]·H2O (3), in which dimethylammonium replaces ammonium cations, crystallizes as a two-dimensional network with honeycomb {63} topology, albeit with very distorted, elongated hexagonal cells. These and previous results show that both NH4+ and PPh4+ or PPh3Me+ cations are essential to the formation of the metallatricycle. The role of the flexibility imparted to ADA2- by the acetate arms, in comparison to the more rigid 1,3-adamantanedicarboxylate (ADC2-), is also discussed. All three complexes are luminescent, with quantum yields of 0.06, 0.06, and 0.09 for 1-3, respectively. The vibronic fine structure apparent on the emission spectra gives peak positions typical of species in which the uranyl ion is chelated by three carboxylate groups.

Chemicals Related in the Paper:

Catalog Number	Product Name	Structure	CAS Number	Price
AP17768284	1,3-Adamantanediacetic acid		17768-28-4	Price

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