Interaction of actinides with aluminosilicate colloids in statu nascendi: Part II: spectroscopic speciation of colloid-borne actinides(III)

作者: P.J. Panak , M.A. Kim , J.I. Yun , J.I. Kim

DOI: 10.1016/S0927-7757(03)00351-0

关键词:

摘要: Abstract The chemical interaction of trivalent actinides, Am(III) and Cm(III) in the process hydroxy aluminosilicate (HAS) colloid formation is investigated by time-resolved laser fluorescence spectroscopy (TRLFS) with assistance radiometry. A screening experiment performed at beginning to ascertain under what conditions HAS colloids are formed favourably incorporate actinides their oxo-bridge structure. While keeping Si concentration constant 10−3 mol l−1, Al varied from 10−7 l−1 pH range 4 9. electrolyte medium made 0.03 M NaCl. trace amount 241Am or 248Cm introduced a 4.9×10−8 l−1. favourable condition as ascertained radiometric found be around 5 10−6–10−5 for marginal pH≥7 10−6–10−4 major amount. Spectroscopic speciation on Cm, its high yield, various experimental solutions appraisal binding within oxo-bridges colloids. Speciation TRLFS shows two colloid-borne Cm species, Cm-HAS(I) Cm-HAS(II), which have seven six hydration water molecules, respectively. These results put forward conclusion that former undergoes bidentate latter tridentate binding. In absence Al, reaction silanol moieties form Cm–silicate complexes, distributed three phases: ionic phase, precipitate. However, due low concentration. Applying laser-induced breakdown detection (LIBD), an average size 11–13 nm hard sphere diameter different pH.

参考文章(36)
Robert E. Mesmer, Charles F. Baes, The hydrolysis of cations ,(1976)
W. Hauser, H. Geckeis, J.I. Kim, Th. Fierz, A mobile laser-induced breakdown detection system and its application for the in situ-monitoring of colloid migration Colloids and Surfaces A: Physicochemical and Engineering Aspects. ,vol. 203, pp. 37- 45 ,(2002) , 10.1016/S0927-7757(01)01086-X
C. Walther, C. Bitea, W. Hauser, J.I. Kim, F.J. Scherbaum, Laser induced breakdown detection for the assessment of colloid mediated radionuclide migration Nuclear Instruments & Methods in Physics Research Section B-beam Interactions With Materials and Atoms. ,vol. 195, pp. 374- 388 ,(2002) , 10.1016/S0168-583X(02)01128-X
Thorsten Stumpf, Andreas Bauer, Frederic Coppin, Jae Il Kim, Time-resolved laser fluorescence spectroscopy study of the sorption of Cm(III) onto smectite and kaolinite. Environmental Science & Technology. ,vol. 35, pp. 3691- 3694 ,(2001) , 10.1021/ES001995O
Claude Degueldre, Iñes Triay, Jae-Il Kim, Peter Vilks, Marcus Laaksoharju, Norbert Miekeley, Groundwater colloid properties: a global approach Applied Geochemistry. ,vol. 15, pp. 1043- 1051 ,(2000) , 10.1016/S0883-2927(99)00102-X
M. Bouby, T. Ngo Manh, Horst Geckeis, Franz J. Scherbaum, Jae-Il Kim, Characterization of aquatic colloids by a combination of LIBD and ICP-MS following the size fractionation Radiochimica Acta. ,vol. 90, pp. 727- 732 ,(2002) , 10.1524/RACT.2002.90.9-11_2002.727
William L. Bourcier, Kevin G. Knauss, Kenneth J. Jackson, Aluminum hydrolysis constants to 250°C from boehmite solubility measurements Geochimica et Cosmochimica Acta. ,vol. 57, pp. 747- 762 ,(1993) , 10.1016/0016-7037(93)90166-T
Takaumi Kimura, Gregory R. Choppin, Luminescence study on determination of the hydration number of Cm(III) Journal of Alloys and Compounds. ,vol. 213, pp. 313- 317 ,(1994) , 10.1016/0925-8388(94)90921-0
M. Plaschke, T. Schäfer, T. Bundschuh, T. Ngo Manh, R. Knopp, H. Geckeis, J. I. Kim, Size characterization of bentonite colloids by different methods. Analytical Chemistry. ,vol. 73, pp. 4338- 4347 ,(2001) , 10.1021/AC010116T
Thomas Rabung, Thorsten Stumpf, Horst Geckeis, R. Klenze, J. I. Kim, Sorption of Am(III) and Eu(III) onto γ-alumina: experiment and modelling Radiochimica Acta. ,vol. 88, pp. 711- 716 ,(2000) , 10.1524/RACT.2000.88.9-11.711