Molecular and polymeric uranyl and thorium hybrid materials featuring methyl substituted pyrazole dicarboxylates and heterocyclic 1,3-diketones

Korey P Carter; Andrew T Kerr; Ilya V Taydakov; Christopher L Cahill

doi:10.1016/j.solidstatesciences.2017.12.002

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Molecular and polymeric uranyl and thorium hybrid materials featuring methyl substituted pyrazole dicarboxylates and heterocyclic 1,3-diketones

Journal article

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Molecular and polymeric uranyl and thorium hybrid materials featuring methyl substituted pyrazole dicarboxylates and heterocyclic 1,3-diketones

Korey P Carter, Andrew T Kerr, Ilya V Taydakov and Christopher L Cahill

Solid state sciences, Vol.76(C), pp.20-32

02/2018

DOI: 10.1016/j.solidstatesciences.2017.12.002

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Abstract

A series of seven novel f-element bearing hybrid materials have been prepared from either methyl substituted 3,4 and 4,5-pyrazoledicarboxylic acids, or heterocyclic 1,3- diketonate ligands using hydrothermal conditions. Compounds 1, [UO2(C6H4N2O4)2(H2O)], and 3, [Th(C6H4N2O4)4(H2O)5]·H2O feature 1-Methyl-1H-pyrazole-3,4-dicarboxylate ligands (SVI-COOH 3,4), whereas 2, [UO2(C6H4N2O4)2(H2O)], and 4, [Th(C6H5N2O4)(OH)(H2O)6]2·2(C6H5N2O4)·3H2O feature 1-Methyl-1H-pyrazole-4,5-dicarboxylate moieties (SVI-COOH 4,5). Compounds 5, [UO2(C13H15N4O2)2(H2O)]·2H2O and 6, [UO2(C11H11N4O2)2(H2O)]·4.5H2O feature 1,3-bis(4-N1-methyl-pyrazolyl)propane-1,3-dione and 1,3-bis(4-N1,3-dimethyl-pyrazolyl)propane-1,3-dione respectively, whereas the heterometallic 7, [UO2(C11H11N4O2)2(CuCl2)(H2O)]·2H2O is formed by using 6 as a metalloligand starting material. Single crystal X-ray diffraction indicates that all coordination to either [UO2]2+ or Th(IV) metal centers is through O-donation as anticipated. Room temperature, solid-state luminescence studies indicate characteristic uranyl emissive behavior for 1 and 2, whereas those for 5 and 6 are weak and poorly resolved. A series of seven novel f-element bearing hybrid materials have been prepared from either methyl substituted 3,4 and 4,5-pyrazoledicarboxylic acids, or heterocyclic 1,3- diketonate ligands using hydrothermal conditions. [Display omitted] •Seven novel 5f hybrid materials have been prepared.•Uranyl compounds containing methyl substituted 3,4 and 4,5-pyrazoledicarboxylate ligands feature typical uranyl emission.•Novel methyl substituted pyrazole dicarboxylates and heterocyclic 1,3-diketones feature multiple H-bonding synthon sites.

Details

Title: Subtitle: Molecular and polymeric uranyl and thorium hybrid materials featuring methyl substituted pyrazole dicarboxylates and heterocyclic 1,3-diketones
Creators: Korey P Carter - Department of Chemistry, The George Washington University, 800 22nd Street, NW, Suite 4000, Washington, D.C. 20052, United States
Andrew T Kerr - Department of Chemistry, The George Washington University, 800 22nd Street, NW, Suite 4000, Washington, D.C. 20052, United States
Ilya V Taydakov - P. N. Lebedev Institute of the Russian Academy of Sciences, Leninskiy Prospect, 53, Moscow 119991, Russian Federation
Christopher L Cahill - Department of Chemistry, The George Washington University, 800 22nd Street, NW, Suite 4000, Washington, D.C. 20052, United States
Resource Type: Journal article
Publication Details: Solid state sciences, Vol.76(C), pp.20-32
DOI: 10.1016/j.solidstatesciences.2017.12.002
ISSN: 1293-2558
eISSN: 1873-3085
Publisher: Elsevier Masson SAS
Grant note: DOI: 10.13039/100006151, name: U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, award: DE-SC0001089; DOI: 10.13039/100007108, name: George Washington University
Language: English
Date published: 02/2018
Academic Unit: Chemistry
Record Identifier: 9984216603102771

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