Liquid chromatographic studies on the behaviour of Pu(III), Pu(IV) and Pu(VI) on a RP stationary phase in presence of α-Hydroxyisobutyric acid as a chelating agent
-
P.G. Jaison
,
Pranaw Kumar
Abstract
Since plutonium possesses multiple oxidation states which can coexist in solution, a method for the identification of these oxidation states is important to understand its chemical processes. Liquid chromatographic studies were carried out to compare the chromatographic behaviour of different oxidation states of Pu in presence of the eluent, α-hydroxyisobutyric acid (HIBA). The three oxidation states of Pu viz. Pu(III), Pu(IV) and Pu(VI) were separated under optimised conditions. It was seen that the presence of the complexing agent influences the equilibrium of Pu(III)/(IV) as well as Pu(IV)/(VI) systems. Pu(III) to Pu(IV) conversion was found to be enhanced by high pH and concentration of HIBA whereas a relatively low pH and high concentration of HIBA promotes the conversion of Pu(VI) to Pu(IV).
Acknowledgments
Authors are thankful to Dr. K. L. Ramakumar, Director, Radiochemistry and Isotope Group, BARC, Dr. S. Kannan, Head, Fuel Chemistry Division and Dr. D. Alamelu, Head, Mass Spectrometry Section for their support and encouragements. We gratefully acknowledge the help provided by Dr. M. K. Sharma and Mr. R. Agarwal for the electrochemical preparation of Pu in different oxidation states. Authors would also like to thank Mr. A. S. Kanekar for UV-Vis spectrophotometry measurements. Special thanks are due to Dr. S. Chaudhury and Mr. S. Pathak for their support in the sample preparations.
References
1. Qiao, J., Hou, X., Miro, M., Roos, P.: Determination of plutonium isotopes in waters and environmental solids: A review. Anal. Chim. Acta 652, 66 (2009).10.1016/j.aca.2009.03.010Suche in Google Scholar
2. Morss, L. R., Edelstein, N. M., Fuger, J.: The chemistry of the actinide and transactinide elements, 4th ed., Springer, The Netherlands (2010), p. 1117.10.1007/978-94-007-0211-0Suche in Google Scholar
3. Ekberg, C., Larsson, K., Skarnemark, G., Odegaard-Jensen, A., Persson, I.: The structure of plutonium(IV) oxide as hydrolysed clusters in aqueous suspensions. Dalton Trans. 42, 2035 (2013).10.1039/C2DT32185HSuche in Google Scholar
4. Clark, D. L.: The chemical complexities of plutonium. Los Alamos Sci. 26, 364 (2000).Suche in Google Scholar
5. Graser, C. H., Banik, N. L., Bender, K. A., Lagos, M., Marquardt, C. M., Marsac, R., Montoya, V., Geckeis, H.: Sensitive redox speciation of iron, neptunium, and plutonium by capillary electrophoresis hyphenated to inductively coupled plasma sector field mass spectrometry. Anal. Chem. 87, 9786 (2015).10.1021/acs.analchem.5b02051Suche in Google Scholar
6. Fujiwara, K., Yamana, H., Fujii, T., Moriyama, H.: Solubility product of plutonium hydrous oxide. J. Nucl. Fuel. Cycle Environ. 7, 17 (2001).10.1524/ract.2002.90.12_2002.857Suche in Google Scholar
7. Walther, C., Rothe, J., Fuss, M., Buchner, S.: A link between the oxidation states? Colloids and mixed-valence polymers of plutonium in aqueous solution. ARQ 17, 19 (2009).Suche in Google Scholar
8. Lloyd, M. H., Haire, R. G.: Chemistry of plutonium in sol-gel processes. Radiochim. Acta 25, 139 (1978).10.1524/ract.1978.25.34.139Suche in Google Scholar
9. Neck, V., Altmeier, M., Seibert, A. Yun, J. I., Marquardt, C. M., Fanghänel, T.: Solubility and redox reactions of Pu (IV) hydrous oxide: evidence for the formation of PuO2+ x(s, hyd). Radiochim. Acta 95, 193 (2007).10.1524/ract.2007.95.4.193Suche in Google Scholar
10. Luksiene, B., Druteikiene, R., Peciulyte, D., Baltrunas, D., Remeikis, V., Paskevicius, A.: Effect of microorganisms on the plutonium oxidation states. Appl. Radiat. Isot. 70, 442 (2012).10.1016/j.apradiso.2011.11.016Suche in Google Scholar
11. Silver, G. L.: Plutonium oxidation states in seawater. Appl. Radiat. Isot. 55, 589 (2001).10.1016/S0969-8043(01)00097-5Suche in Google Scholar
12. Simpson, M. F., Law, J. D.: Nuclear Fuel Reprocessing. Idaho National Laboratory Report INL/EXT-10-17753 (2010).Suche in Google Scholar
13. Wilson, R. E., Hu, Y. J., Nitsche, H.: Low-level detection and quantification of plutonium (III, IV, V, and VI) using a liquid core waveguide. Plutonium Futures – The Science Conference Albuquerque, NM, USA July 6–10, 2003.10.1063/1.1594570Suche in Google Scholar
14. Nitsche, H., Lee, S. C., Gatti, R. C.: Determination of plutonium oxidation states at trace levels pertinent to nuclear waste disposal. J. Radioanal. Nucl. Chem. 124, 171 (1988).10.1007/BF02035515Suche in Google Scholar
15. Gehmecker, H.; Trautmann, N.; Herrmann, G.: Separation of plutonium oxidation states by ion exchange chromatography. Radiochim. Acta 40, 81 (1986).10.1524/ract.1986.40.2.81Suche in Google Scholar
16. Burger, S., Banik, N. L., Buda, R. A., Kratz, J. V., Kuczewski, B., Trautmann, N.: Speciation of the oxidation states of plutonium in aqueous solutions by UV/Vis spectroscopy. Radiochim. Acta 95, 433 (2007).10.1524/ract.2007.95.8.433Suche in Google Scholar
17. Panak, P. J., Booth, C. H., Caulder, D. L., Bucher, J. ., Shuh, D. K., Nitsche, H.: X-ray absorption fine structure spectroscopy of plutonium complexes with bacillus sphaericus. Radiochim. Acta 90, 315 (2002).10.1524/ract.2002.90.6.315Suche in Google Scholar
18. Kumar, P., Paul, S., Jaison, P. G., Telmore, V. M., Alamelu, D., Aggarwal, S. K.: HPLC method for determination of Th, U and Pu in irradiated (Th,Pu)O2 using mandelic acid as an eluent. Radiochim. Acta 102, 973 (2014).10.1515/ract-2013-2242Suche in Google Scholar
19. Gunther, I. L., Waldis, J. K., Wernli, B., Kopajtic, Z.: Measurement of plutonium isotope ratios in nuclear fuel samples by HPLC-MC-ICP-MS. Int. J. Mass Spectrom. 242, 197 (2005).10.1016/j.ijms.2004.11.007Suche in Google Scholar
20. Sivaraman, N., Subramaniam, S., Srinivasan, T. G., Rao, P. R. V.: Burn-up measurements on nuclear reactor fuels using high performance liquid chromatography. J. Radioanal. Nucl. Chem. 253, 35 (2002).10.1023/A:1015800114488Suche in Google Scholar
21. Datta, A., Sivaraman, N., Viswanathan, K. S., Ghosh, S., Srinivasan, T. G., Rao, P. R. V.: Correlation of retention of lanthanide and actinide complexes with stability constants and their speciation. Radiochim. Acta 101, 81 (2013).10.1524/ract.2013.2005Suche in Google Scholar
22. Fedoseev, A. M., Gogolev, A. V., Shilov, V. P.: Reduction of Np(VI) and Pu(VI) with anions of some substituted carboxylic acids. Radiochemistry 55, 155 (2013).10.1134/S1066362213020033Suche in Google Scholar
23. Ryan, J. L., Wheelwright, E. J.: Recovery and purification of plutonium by anion exchange. Ind. Eng. Chem. 51, 60 (1959).10.1021/ie50589a038Suche in Google Scholar
24. Manolkar, R. B., Chander, K., Marathe, S. G.; Alpha-liquid scintillation counting for the determination of plutonium. J. Radioanal. Nucl. Chem., 177, 373, (1994).10.1007/BF02061134Suche in Google Scholar
25. Lumetta G. J., Delegard, C. H., Meier, D. E., Edwards, M. K., Tingey, J. M., Jones, S. A., Casella, A. J., Rapko, B. M.: Conceptual design for the pilot-scale plutonium oxide processing unit in the radiochemical processing laboratory, Technical Report No. PNNL-23534 (2014).10.2172/1160202Suche in Google Scholar
26. Silver, G. L.: Determination of plutonium oxidation states in dilute nitric acid by complementary tristimulus colorimetry. Talanta 14, 637 (1967).10.1016/0039-9140(67)80030-4Suche in Google Scholar
27. Jaison, P.G., Raut, N. M., Aggarwal, S. K.: Direct determination of lanthanides in simulated irradiated thoria fuels using reversed-phase high-performance liquid chromatography. J. Chromatogr. A 1122, 47 (2006).10.1016/j.chroma.2006.04.037Suche in Google Scholar PubMed
28. Lough, W. J., Wainer, I. W.: High performance liquid chromatography: fundamental principles and practice, Blackie Academic & Professional, Glasgow (1995), p. 168.Suche in Google Scholar
29. Boukhalfa, H., Icopini, G. A., Reilly, S. D., Neu, M. P.: Plutonium(IV) reduction by the metal-reducing bacteria Geobacter metallireducens GS15 and Shewanella oneidensis MR1. Appl. Environ. Microbiol. 73, 5897 (2007).10.1128/AEM.00747-07Suche in Google Scholar PubMed PubMed Central
30. AlMahamid, I., Becraft, K. A., Hakem, N. L., Gatti, R. C., Nitsche, H.: Stability of various plutonium valence states in the presence of NTA and EDTA. Radiochimica Acta 74, 129 (1996).10.1524/ract.1996.74.special-issue.129Suche in Google Scholar
©2017 Walter de Gruyter GmbH, Berlin/Boston
Artikel in diesem Heft
- Frontmatter
- Preface
- Separation Science and Technology in India
- Separation of americium (III) and strontium (II) using TEHDGA and 18-crown-6
- Diglycolic acid modified zirconium phosphate and studies on the extraction of Am(III) and Eu(III) from dilute nitric acid medium
- Extraction of plutonium(IV) by diglycolamide extractants in room temperature ionic liquids
- Liquid chromatographic studies on the behaviour of Pu(III), Pu(IV) and Pu(VI) on a RP stationary phase in presence of α-Hydroxyisobutyric acid as a chelating agent
- Evaluation of several novel diamide based ligands for selective extraction of tetravalent plutonium
- Redox speciation of uranium with phenylphosphonic acid (PPA) in aqueous medium
- Third phase formation in the extraction of Th(NO3)4 by Tri-sec-butyl phosphate: a comparison with Tri-n-butyl phosphate
- Experimental and theoretical studies on extraction of actinides and lanthanides by alicyclic H-phosphonates
- Removal of radiocesium from low level radioactive effluents by hexacyanoferrate loaded synthetic zeolite: laboratory to pilot plant scale demonstration
Artikel in diesem Heft
- Frontmatter
- Preface
- Separation Science and Technology in India
- Separation of americium (III) and strontium (II) using TEHDGA and 18-crown-6
- Diglycolic acid modified zirconium phosphate and studies on the extraction of Am(III) and Eu(III) from dilute nitric acid medium
- Extraction of plutonium(IV) by diglycolamide extractants in room temperature ionic liquids
- Liquid chromatographic studies on the behaviour of Pu(III), Pu(IV) and Pu(VI) on a RP stationary phase in presence of α-Hydroxyisobutyric acid as a chelating agent
- Evaluation of several novel diamide based ligands for selective extraction of tetravalent plutonium
- Redox speciation of uranium with phenylphosphonic acid (PPA) in aqueous medium
- Third phase formation in the extraction of Th(NO3)4 by Tri-sec-butyl phosphate: a comparison with Tri-n-butyl phosphate
- Experimental and theoretical studies on extraction of actinides and lanthanides by alicyclic H-phosphonates
- Removal of radiocesium from low level radioactive effluents by hexacyanoferrate loaded synthetic zeolite: laboratory to pilot plant scale demonstration
