From Layered Structures to Cubic Frameworks: Expanding the Structural Diversity of Uranyl Carboxyphosphonates via the Incorporation of Cobalt

Alsobrook, A. N., Hauser, B. G., Hupp, J. T., Aekseev, E. V., Depmeier, W. and Albrecht-Schmitt, T. E. (2011) From Layered Structures to Cubic Frameworks: Expanding the Structural Diversity of Uranyl Carboxyphosphonates via the Incorporation of Cobalt Crystal Growth & Design, 11 (4). pp. 1385-1393. DOI 10.1021/c9101668f.

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Abstract

Five heterobimetallic U(VI)/Co(II) carboxyphosphonates have been synthesized under mild hydrothermal conditions by reacting UO(3), Co(CH(3)CO(2))(2)center dot 4H(2)O, and triethyl phosphonoacetate. These compounds, Co(H(2)O)(4)[(UO(2))(2)(PO(3)CH(2)CO(2))(2)(H(2)O)(2)] (CoUpAA-1), [Co(H(2)O)(6)][UO(2)(PO(3)CH(2)CO(2))](2)center dot 8H(2)O (CoUPAA-2), Co(H(2)O)(4)UO(2)(PO(3)CH(2)CO(2))](2)center dot 4H(2)O (CoUPAA-3), Co(H(2)O)(4)[(UO(2))(6)(PO(3)CH(2)CO(2))(2)O(2)(OH)(3)(H(2)O)(3)]2 center dot 3H(2)O (CoUPAA-4), and Co(2)[(UO(2))(6)(PO(3)CH(2)CO(2))(3)O(3)(OH)(H(2)O)(2)]center dot 16H(2)O (CoUPAA-5), range from two- to three-dimensional structures. CoUPAA-1 to CoUPAA-3 all possess uranyl carboxyphosphonate layers that are separated by the Co(II) cation with varying degrees of hydration. CoUPAA-4 contains both UO(7) pentagonal bipyramids and UO(8) hexagonal bipyramids within the uranyl carboxyphosphonate plane. Unlike the first four low-symmetry compounds, CoUPAA-5 is a cubic, three-dimensional network with large cavities approximately 16 A in diameter that are filled with cocrystallized water molecules. Differential gas absorption measurements performed on CoUPAA-5 displayed a surface area uptake for CO(2) of 40 m(2) g(-1) at 273 K, and no uptake for N(2) at 77 K.

Document Type: Article
Keywords: cation-cation interactions bond-valence parameters uranium(vi) carboxyphosphonates crystal-structures nuclear-waste ion-exchange u6+ minerals neptunium insights thorium
Research affiliation: Kiel University
DOI etc.: 10.1021/c9101668f
ISSN: 1528-7483
Date Deposited: 15 Dec 2011 05:27
Last Modified: 08 Oct 2012 09:26
URI: http://eprints.uni-kiel.de/id/eprint/15608

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