Structural studies on the actinide carboxylates—IV The crystal and molecular structure of succinate dioxouranium(VI) monohydrate

doi:10.1016/0022-1902(79)80513-8

Journal of Inorganic and Nuclear Chemistry

Volume 41, Issue 2, 1979, Pages 201-203

https://doi.org/10.1016/0022-1902(79)80513-8 Get rights and content

Abstract

The structure of the title compound, UO₂(CH₂COO)₂·H₂O, has been determined from three-dimensional X-ray data. The crystals are orthorhombic, space group Pbcn with four formula units in a cell of dimensions $a = 7.583(2), b = 9.491(3) and c = 10.890(3) A ̊$ . Least-squares refinement has led to a value of the conventional R index of 0.039 for the 418 unique reflections having I⩾3σ(I). The coordination geometry about the uranium atom is pentagonal bipyramidal. The uranyl ions are equatorially surrounded by one water oxygen and by four carboxylate oxygen atoms of different succinic ligands. Each ligand is shared by four uranyl units giving rise to a polymeric-like structure.

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Potassium and magnesium succinatouranilates – Synthesis and crystal structure
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It is typical of malonate (m=1) and succinate (m=2) compounds of U(6+) to have o large (few decades) time gap between the first and the following publications on crystal structures. To date, crystallographic data on twelve uranium succinate compounds are available [8–13]. Three of them are based on 3D frameworks, which are less common, compare to 1D and 2D units in crystal structures of U(VI) compounds [14].
Single crystal X-ray diffraction has been applied to determine the structures of two new uranyl coordination polymers: K₂[(UO₂)₂(C₄H₄O₄)₃] (1) and [Mg(H₂O)₆] [(UO₂)₂(C₄H₄O₄)₃]·2H₂O (2), where C₄H₄O₄^2- is succinate anion. Crystals of 1 and 2 contain polymeric complex anions [(UO₂)₂(C₄H₄O₄)₃]^2- with the same A₂Q⁰²₃ crystallochemical formula (A=UO₂²⁺, Q⁰²=C₄O₄H₄^2-), and have layered (1) or chain (2) structure. It has been found, that conformation of succinate ions is one of the factors, which affects the structure of [(UO₂)₂(C₄H₄O₄)₃]^2- anions. IR spectra of these new compounds are in good agreement with crystallographic data. Topological analysis of the uranium dicarboxylates with A₂Q⁰²₃ crystallochemical formula has shown the presence of five isomers which differ from each other in coordination sequences and / or dimensionality.
Unexpected cis-dioxido uranyl carboxylate compound: Synthesis, characterization and photocatalytic activity of uranyl-succinate complexes
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Two new complexes formed by uranyl ions with succinic acid and 4,4′-dipyridine have been investigated. Interestingly, the uranium(VI) coordination polymers possess two types dioxido unit, a cis-dioxido bond angle with 115.421(2)°and a trans-dioxido bond angle with 178.421(2)°, respectively. The complexes were characterized by elemental analysis, IR and UV–vis spectroscopy and X-ray crystal diffraction. In addition, the properties of luminescence and photocatalytic analysis were also investigated. The result revealed that the two complexes show different photocatalytic activity in the decomposition of RhB under visible light and UV light irradiation.
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The EDS ligands coordinate in a bridging bidentate fashion to yield neutral chains. Comparing this structure type to those formed by similarly sized phosphonate (ethylenediphosphonic acid) (Tian et al., 2013a) and carboxylate (succinic acid) (Bombieri et al., 1979) linkers one can observe an overall difference in both connectivity and resulting dimensionality. The phosphonate linkers coordinated in a multidentate fashion and gave rise to a 2D layered topology, whereas the carboxylate linkers coordinated via bridging bidentate to yield an overall 3D framework.
The structural chemistry of crystalline hybrid materials bearing the uranyl cation, [UO₂]^2 +, is reviewed. A theme of uranyl hydrolysis and complex aqueous speciation as drivers for structural diversity is developed for materials constructed from coordinate covalent bonding with various O- and N-donor ligands. We begin with results from a number of exploratory hydrothermal synthesis efforts to highlight structural themes dominated by oligomeric secondary building units, and ligand affinities and sterics. The review then evolves to highlight more focused studies that endeavor to promote incorporation of targeted coordination geometries, compositions, and connectivities. Finally, we explore purely supramolecular systems that focus on the assembly of specific uranyl-bearing ions such as [UO₂X₄(H₂O)_n]^2 − (X = Cl, Br) and [UO₂(NCS)_5 − n(H₂O)n] (n = 0, 1) formed from high anion media. Assembly of these tectons is afforded through noncovalent interactions (synthons) with appropriate organic molecules to promote hydrogen or halogen bonding. The luminescent behavior of selected compounds is presented where clear structure–property relationships may be discerned.
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Others with distinct ratio of 1, are negatively charged entities and having as counter-ion metallic cations or protonated organic bases. Only two complexes exhibit a three-dimensional framework, with the succinate (C2) and sebacate (C5) in [UO2(suc)(H2O)] [22,176] and [(UO2)2(H2O)(sbc)2(edpy)] [177], respectively. The second and most prolific category contains aliphatic linear or cyclic, mono- or polycarboxylates (Table 5).
The field of uranium carboxylates has been studied for several decades and an important library of coordination complexes and network solids is now well defined. It mainly concerns the reactivity of hexavalent uranium (uranyl) with the different types of carboxylic acids containing monodentate or polydentate functions, aliphatic or aromatic carbon backbone, or hetero-systems offering other functionalities (N-donor, S-donor, phosphonates, …). A rich variety of molecular complexes or extended multi-dimensional networks (1D, 2D, 3D) has been identified and depends mainly on the equatorial connectivity of the uranyl cation (UO₂²⁺) in different coordination numbers (tetragonal, pentagonal or hexagonal bipyramid). The yl oxo groups remain relatively inert to condensation process (except rare case of cation–cation interaction). For lower oxidation state of uranium (+3, +4, +5), the knowledge is at the infancy stage since very few contributions are available in literature. Nevertheless, recent contributions have shown the possibilities of the reactivity of tetravalent uranium in relatively stable architectures, either at the molecular level, with high nuclearities (up to U₃₈), or engaged in three-dimensional frameworks. The scope of this review is a comprehensive presentation of the crystal structures resulting from the different types of complexation of uranium with carboxylic acid molecules (excepting oxalate ligand) and their classification as a function of the nuclearity of identified building units.
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New Uranyl Succinate-Containing Polymers: Synthesis and Structure
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Structural studies on the actinide carboxylates—IV The crystal and molecular structure of succinate dioxouranium(VI) monohydrate

Abstract

J. Inorg. Nucl. Chem.

An. Quim.

An. Quim.

Acta Cryst.

Acta Cryst.

Jahresb der Chemie