Abstract
This study mainly focuses hydrolysis reactions of uranium(VI) under an ambient atmosphere leading to colloid formation in near neutral solution using light scattering, UV–Vis and FTIR-ATR studies. UV–Vis and IR spectrum was recorded for uranyl solution at different pH range. U(VI) hydrolyzed colloids were detected and it was confirmed by the appearance of a band at 941 cm−1 in the IR spectra. Light scattering measurements were performed on colloidal U(VI) solutions formed at pH range of 7–8. The average particle diameter was determined as 32–36 nm using dynamic light scattering. Well defined colloidal species are formed with no considerable change in particle size with increasing U(VI) concentration. The weight average molecular weight of colloidal species was predicted as 763 Da by Debye plot. The second virial coefficient (A2) was found to be −0.1139 ml g−1 Da. The present study confirms that behaviour of U(VI) contradicts conventional Zr(IV), Th(IV) and Pu(IV) solution chemistry. U(VI) polymerization is less extensive and in neutral solutions it forms only oligomers with 2–3 uranyl units.
References
Neck V, Kim JI (2001) Solubility and hydrolysis of tetravalent actinides. Radiochim Acta 89:1–16. doi:10.1524/ract.2001.89.1.001
Torapava N, Persson I, Eriksson L, Lundberg D (2009) Hydration and hydrolysis of Th(IV) in aqueous solution and the structures of two crystalline Th(IV) hydrates. Inorg Chem 48:11712–11723. doi:10.1021/ic901763s
Altmaier M, Gaona X, Fanghanel T (2013) Recent advances in aqueous actinide chemistry and thermodynamics. Chem Rev 113:901–943. doi:10.1021/cr300379w
Bhandari D, Wells SM, Retterer ST, Sepaniak MJ (2009) Characterization and detection of uranyl ion sorption on silver surfaces using surface enhanced Raman Spectroscopy. Anal Chem 81:8061–8067. doi:10.1021/ac901266f
Zanker H, Kai-Uwe Ulrich, Opel K, Brendler V (2007) The role of colloids in uranium transport: a comparison of nuclear waste repositories and abandoned uranium mines. In: Cidu R, Frau F (eds) IMWA symposium, Water in mining environments, Italy. http://www.imwa.info/docs/imwa_2007/IMWA2007_Zaenker.pdf, Accessed 30 Apr 2013
Zhao P, Steward SA (1997) Literature review of intrinsic actinide colloids related to spent fuel waste package release rates. Lawrence Livermore National laboratory. doi:10.2172/461376
Guillaumont R, Fanghanel T, Fuger J, Grenthe L, Neck V, Palmer DA, Rand MH (2003) Update on the chemical thermodynamics of Uranium, Neptunium, Plutonium. Americium and Technicium, North-Holland
Eliet V, Bidoglio G (1998) Kinetics of the laser-induced photoreduction of U(VI) in aqueous suspensions of TiO2 particles. Environ Sci Technol 32:3155–3161. doi:10.1021/es970929s. http://lib3.dss.go.th/fulltext/Journal/Environ%20Sci.%20Technology1998-2001/1998/no.20/20,1998%20vol.32,no.20,p3155-3161.pdf. Accessed 30 Apr 2013
Clark DL, Conradson SD, Donohoe RJ, Webster Keogh D, Morris DE, Palmer PD, Rogers RD, Drew Tait C (1999) Chemical speciation of the uranyl ion under highly alkaline conditions. Synthesis, structures and oxo ligand exchange dynamics. Inorg Chem 38:1456–1466. doi:10.1021/ic981137h
Steppert M, Walther C, Fuss M, Buchner S (2012) On the polymerization of hexavalent Uranium. An electrospray mass spectrometry study. Rapid Commun Mass Spectrom 26:583–591. doi:10.1002/rcm.6128
Palmer DA, Nguyen-Trung C (1995) Aqueous uranyl complexes. 3. Potentiometric measurements of the hydrolysis of uranyl(VI) ion at 25 °C. J Solution Chem 24:1281–1291. doi:10.1007/BF00972833
Eliet V, Grenthe I, Bidoglio G (2000) Time-resolved laser-induced fluorescence of uranium(VI) hydroxo-complexes at different temperatures. Appl Spectrosc 54:99–105. doi:10.1366/0003702001948178
Toth LM, Begun GM (1981) Raman spectra of uranyl ion and its hydrolysis products in aqueous HNO3. J Phys Chem 85:547–549. doi:10.1021/j150605a018
Quiles F, Burneau A (1998) Infrared and Raman spectroscopic study of uranyl complexes: hydroxide and acetate derivatives in aqueous solution. Vib Spectrosc 18:61–75. doi:10.1016/S0924-2031(98)00040-X
Quiles F, Burneau A (2000) Infrared and Raman spectra of uranyl(VI) oxo-hydroxo complexes in acid aqueous solutions: a chemometric study. Vib Spectrosc 23:231–241. doi:10.1016/S0924-2031(00)00067-9
Muller K, Brendler V, Foerstendorf H (2008) Aqueous Uranium(VI) hydrolysis species characterized by attenuated total reflection Fourier-Transform Infrared spectroscopy. Inorg Chem 21:10127–10134. doi:10.1021/ic8005103
Bullock JI (1967) Infrared spectra of some uranyl nitrate complexes. J Inorg Nucl Chem 29:2257–2264. doi:10.1016/0022-1902(67)80280-X
Rush RM, Johnson JS, Kraus KA (1961) Hydrolysis of Uranium(VI): ultracentrifugation and acidity measurements in chloride solutions. Inorg Chem 1:378–386. doi:10.1021/ic50002a036
Lubal P, Havel J (1997) Spectrophotometric and potentiometric study of Uranyl hydrolysis in perchlorate medium. Is derivative spectrophotometry suitable for search of the chemical model? Chem Papers 51:213–220. http://www.chempap.org/file_access.php?file=514a213.pdf. Accessed 30 Apr 2013
Redkin AF, Wood SA (2007) Uranium(VI) in aqueous solutions at 25 °C and a pressure of 1 bar: insight from experiments and calculations. Geochem Int 45:1111–1123. doi:10.1134/S0016702907110043
Kirishima A, Kimura T, Tochiyama O, Yoshida Z (2004) Speciation study on uranium(VI) hydrolysis at high temperatures and pressures. J Alloy Compd 374:277–282. doi:10.1016/j.jallcom.2003.11.105
Brooker MH, Huang CH, Sylwestriwicz J (1979) Raman spectroscopic studies of aqueous uranyl nitrate and perchlorate systems. J Inorg Nucl Chem 42:1431–1440. doi:10.1016/0022-1902(80)80109-6
Urban C, Peter S (1998) Characterization of turbid colloidal suspensions using light scattering techniques combined with cross correlation methods. J Coll Interface Sci 207:150–158. doi:10.1006/jcis.1998.5769
Priyadarshini N, Sampath M, Kumar S, Mudali UK, Natarajan R (2013) Light scattering studies to determine molecular weight of freshly prepared Zr(IV) hydrous polymer. J Radioanal Nucl Chem 293:1093–1096. doi:10.1007/s10967-012-1951-3
Bonnete F, Finet S, Tardieu A (1999) Second virial coefficient: variations with lysozyme crystallization conditions. J Cryst Growth 196:403–414. doi:10.1016/S0022-0248(98)00826-4
Berne Bruce J, Pecora Robert (1976) Dynamic light scattering with application in physics, chemistry and biology. Wiley, New York
Meinrath G (1997) Uranium(VI) speciation by spectroscopy. J Radioanal Nucl Chem 224:119–126. doi:10.1007/BF02034623
Quiles F, Nguyen-Trung C, Cartret C, Humbert B (2011) Hydrolysis of Uranyl(VI) in acidic and basic aqueous solutions using a noncomplexing organic base: a multivariate spectroscopic and statistical study. Inorg Chem 50:2811–2823. doi:10.1021/ic101953q
Katharina Muller (2010) The sorption of uranium(VI) and neptunium(V) onto surfaces of selected metal oxides and aluminosilicates studied by in situ vibrational spectroscopy. PhD Dessertation, Dresden University. http://www.qucosa.de/fileadmin/data/qucosa/documents/6194/Diss_KaMue_101101.pdf. Accessed 30 Apr 2013
Toth LM, Lin JS, Felker LK (1991) Small angle X-ray scattering from zirconium(IV) hydrous tetramers. J Phys Chem 95:3106–3108. doi:10.1021/j100161a028
Stebbens AE, Shreir LL (1959) Refractive index of Uranium oxide produced by anodic oxidation. Nature 183:1113–1114. doi:10.1038/1831113a0
Ermolaev VM, Zakharova EV, Shilov VP (2001) Depolymerization of Pu(IV) polymer in 0.5–3 M HNO3 in the presence of reductants and oxidants. Radiochemistry 43:424–428. doi:10.1023/A:1012874322870
Rothe J, Walther C, Denecke MA, Fanghanel Th (2004) XAFS and LIBD investigation of the formation and structure of colloidal Pu(IV) hydrolysis products. Inorg Chem 43:4708–4718. doi:10.1021/ic049861p
Toth LM, Friedman HA (1978) The IR spectrum of Pu(IV) polymer. J Inorg Nucl Chem 40:807–810. doi:10.1016/0022-1902(78)80156-0
Ockenden DW, Welch GA (1956) The preparation and properties of some plutonium comounds. V. Colloidal quadrivalent plutonium. J Chem Soc 1:3358–3363. doi:10.1039/JR9560003358
Johnson GL, Toth LM (1978) Plutonium(IV) and Thorium(IV) hydrous polymer chemistry. Technical report ORNL/TM-6365. doi:10.2172/7095381
Thiyagarajan P, Diamond H, Soderholm L, Horwitz, Toth LM, Felker LK (1990) Plutonium(IV) polymers in aqueous and organic media. Inorg Chem 29:1902–1907. doi:10.1021/ic00335a028
Heim K, Foerstendorf (2008) FZD—IRC Annual Report, p 49. http://www.qucosa.de/fileadmin/data/qucosa/documents/2785/12600.pdf. Accessed 30 Apr 2013
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Priyadarshini, N., Sampath, M., Kumar, S. et al. A combined spectroscopic and light scattering study of hydrolysis of uranium(VI) leading to colloid formation in aqueous solutions. J Radioanal Nucl Chem 298, 1923–1931 (2013). https://doi.org/10.1007/s10967-013-2624-6
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-013-2624-6