Molecular Assemblies of a Series of Mixed Tetravalent Uranium and Trivalent Lanthanide Complexes Associated with the Dipicolinate Ligand, in Aqueous MediumClick to copy article linkArticle link copied!
- Nicolas P. MartinNicolas P. MartinUniversité de Lille, Centrale Lille, ENSCL, Univ. Artois, UMR CNRS 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, FranceMore by Nicolas P. Martin
- Christophe VolkringerChristophe VolkringerUniversité de Lille, Centrale Lille, ENSCL, Univ. Artois, UMR CNRS 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, FranceInstitut Universitaire de France (IUF), 1, rue Descartes, 75231 Paris cedex 05, FranceMore by Christophe Volkringer
- Natacha HenryNatacha HenryUniversité de Lille, Centrale Lille, ENSCL, Univ. Artois, UMR CNRS 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, FranceMore by Natacha Henry
- Sylvain DuvalSylvain DuvalUniversité de Lille, Centrale Lille, ENSCL, Univ. Artois, UMR CNRS 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, FranceMore by Sylvain Duval
- Dimitrije MaraDimitrije MaraLuminescent Lanthanide Lab (L3), Department of Chemistry, Ghent University, Krijgslaan 281, S3, 9000 Ghent, BelgiumMore by Dimitrije Mara
- Rik Van DeunRik Van DeunLuminescent Lanthanide Lab (L3), Department of Chemistry, Ghent University, Krijgslaan 281, S3, 9000 Ghent, BelgiumMore by Rik Van Deun
- Thierry Loiseau*Thierry Loiseau*T.L.: e-mail, [email protected]; tel, (33) 3 20 434 122; fax, (33) 3 20 43 48 95.Université de Lille, Centrale Lille, ENSCL, Univ. Artois, UMR CNRS 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, FranceMore by Thierry Loiseau
Abstract
The investigations of the chemical system involving tetravalent uranium associated with trivalent lanthanides (La, Ce, Nd, Sm–Er, Lu) and dipicolinic acid (H2dpa) led to the identification of six distinct types of heterometallic coordination complexes (I–VI). These compounds, obtained at room temperature from aqueous solution, have been characterized by single-crystal X-ray diffraction. They consist of tris-chelated dipicolinate uranium subunits {U(dpa)3} interacting with poly oxo/aquo or mixed polyoxo/aquo chelated dipicolinate lanthanide subunits (LnO1–3(H2O)5–8 or Ln(dpa)O0–3(H2O)4–6) in different arrangements. Complex I (La, Ce) exhibits the assembly of molecular dinuclear [ULn] and [ULnU] trinuclear units, with a linkage between U and Ln via bidentate carboxylate groups of the dipicolinate molecules. The same carboxylate bridging connection mode creates a linear chainlike coordination polymer in complex II (La, Ce), with a strict alternating U–Ln sequence. Complex III (Ce, Nd) contains an octanuclear motif based on six-ring [Ln4U2] decorated by two peripheral {U(dpa)3} subunits, resulting in a [Ln4U4] entity, through carboxylate bridges. Complex IV crystallizes by using a wide series of lanthanide cations (Nd, Sm–Tb) and consists of a simple assembly of discrete {U(dpa)3} subunits with {Ln(Hdpa)(H2O)6}. The complex V (Tb–Er) is composed of a hexanuclear motif based on four-ring [U2Ln2] with two peripheral {U(dpa)3} subunits (final complex [U4Ln2]). The last complex (VI) occurs with the lutetium and is built up from a dinuclear unit [ULu] connected through one carboxylate group. Thermal decomposition of samples of complexes II–IV has been analyzed by thermogravimetry and in situ XRD. The luminescence spectrum of the europium-based complex IV has been measured.
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