title: Synthesis of coffinite, USiO4, and structural investigations of UxTh(1-x)SiO4 solid solutions.
abstract: The miscibility behavior of the USiO4-ThSiO4 system was investigated. The end members and 10 solid solutions UxTh(1-x)SiO4 with x = 0.12-0.92 were successfully synthesized, without formation of other secondary uranium or thorium phases. Lattice parameters of the solid solutions evidently follow Vegard's Law. Investigation of the local structure with EXAFS reveals small differences between the U and Th environment attributed to different atomic radii of the metal atoms but no implications for a miscibility gap. The data provided confirm complete miscibility for the system USiO4-ThSiO4. The structure of the end members was studied in detail with XRD and discussed with special regard to the oxygen positions and the often neglected Si-O bond length. USiO4 could be obtained without UO2 impurities and the lattice parameters derived from Rietveld refinement as c = 6.2606(3) Å and a = 6.9841(3) Å. The Si-O distance in USiO4 appears to be 1.64 Å, which is more reasonable than earlier reported values.
authors.affiliation: Insitute of Energy and Climate Research (IEK-6), Nuclear Waste Management, Forschungszentrum Jülich GmbH , Wilhelm-Johnen-Straße, 54245 Jülich, Germany.
authors.forename: Sabrina
authors.initials: S
authors.lastname: Labs
authors.forename: Christoph
authors.initials: C
authors.lastname: Hennig
authors.forename: Stephan
authors.initials: S
authors.lastname: Weiss
authors.forename: Hilde
authors.initials: H
authors.lastname: Curtius
authors.forename: Harald
authors.initials: H
authors.lastname: Zänker
authors.forename: Dirk
authors.initials: D
authors.lastname: Bosbach
mesh_terms: D018360:Crystallography, X-Ray; D010100:Oxygen / Q000737:chemistry; D017640:Silicates / Q000138:chemical synthesis* / Q000737:chemistry*; D012996:Solutions; D013910:Thorium / Q000737:chemistry*; D014501:Uranium / Q000737:chemistry*; D056928:X-Ray Absorption Spectroscopy; D014961:X-Ray Diffraction
chemical_list: D017640:Silicates; D012996:Solutions; D014501:Uranium; D013910:Thorium; D010100:Oxygen