title: Adsorbed U(VI) surface species on muscovite identified by laser fluorescence spectroscopy and transmission electron microscopy.
abstract: Time-resolved laser-induced fluorescence spectroscopy (TRLFS) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) were applied to investigate the species of uranyl(VI) adsorbed onto muscovite platelets and muscovite suspensions (grain size: 63-200 microm). TRLFS provided evidence for the presence of two adsorbed uranium(VI) surface species on edge-surfaces of muscovite. The two species showed different positions of the fluorescence emission bands and different fluorescence lifetimes indicating a different coordination environment for the two species. HAADF-STEM revealed that nanoclusters of an amorphous uranium phase were attached to the edge-surfaces of muscovite powder during batch sorption experiments. These U-nanoclusters were not observed on {00/} cleavage planes of the muscovite. The surface species with the shorter fluorescence lifetimes are interpreted as truly adsorbed bidentate surface complexes, in which the U(VI) binds to aluminol groups of edge-surfaces. The surface species with the longer fluorescence lifetimes are interpreted to be an amorphous U(VI) condensate or nanosized clusters of polynuclear uranyl(VI) surface species with a particle diameter of 1 to 2 nm. Depending on the size of these clusters the fluorescence lifetimes vary; i.e., the larger the nanosized clusters, the longer is the fluorescence lifetime.
authors.affiliation: FZ Rossendorf e. V., Institute of Radiochemistry, P.O. Box 510119, D-01314 Dresden, Germany. T.Arnold@fz-rossendorf.de
authors.forename: Thuro
authors.initials: T
authors.lastname: Arnold
authors.forename: Satoshi
authors.initials: S
authors.lastname: Utsunomiya
authors.forename: Gerhard
authors.initials: G
authors.lastname: Geipel
authors.forename: Rodney C
authors.initials: RC
authors.lastname: Ewing
authors.forename: Nils
authors.initials: N
authors.lastname: Baumann
authors.forename: Vinzenz
authors.initials: V
authors.lastname: Brendler
mesh_terms: D000327:Adsorption; D000538:Aluminum Silicates / Q000737:chemistry*; D004595:Electroplating / Q000379:methods; D007834:Lasers; D053768:Metal Nanoparticles / Q000032:analysis; D046529:Microscopy, Electron, Transmission / Q000379:methods*; D008903:Minerals / Q000737:chemistry*; D036103:Nanotechnology / Q000379:methods; D011848:Radioactive Pollutants / Q000032:analysis; D013050:Spectrometry, Fluorescence / Q000379:methods*; D014501:Uranium / Q000032:analysis*; D017974:Uranium Compounds / Q000032:analysis
chemical_list: D000538:Aluminum Silicates; D008903:Minerals; D011848:Radioactive Pollutants; D017974:Uranium Compounds; C517971:muscovite; D014501:Uranium