A thermodynamic model of plutonium (IV) nitrate solutions
Tóm tắt
Plutonium nitrate solutions contain a large number of chemical species and they exhibit significant deviations from ideal behavior. Modeling this system is challenging. A model that includes all known chemical species and accounts for nonideal solution behavior could contain several hundred unknown parameters, but insufficient published data exists for evaluating large numbers of parameters. A practical model of plutonium nitrate solutions, therefore, must be a compromise between the number of chemical species included and the number of parameters that can be evaluated from available data. A practical model of acidic plutonium nitrate was developed. The model, which was based on an extended UNIQUAC–Debye–Hückel equation, captures the essential behavior of the system with a minimum number of chemical species. It is capable of representing the vapor–liquid equilibrium data for the nitric acid–water system, the activity of water in the plutonium nitrate-nitric acid–water system, the distribution of plutonium–nitrate complexes in aqueous nitric acid solution, and plutonium adsorption on an anion exchange resin.
Tài liệu tham khảo
Austin G (1984) Shreve’s chemical process industries, 5th edn. McGraw-Hill Book Company, New York
Edwards HGM, Fawcett V (1994) Quantitative Raman spectroscopic studies of nitronium ion concentrations in mixtures of sulphuric and nitric acids. J Mol Struct 326:131–143
Marsh SF, Day RS, Veirs DK (1991) Spectrophotometric investigation of the Pu(IV) nitrate complex sorbed by ion exchange resins. Los Alamos National Laboratory Report LA-12070
Cleveland JM (1967) In: Wick OJ (ed) Plutonium handbook—a guide to the technology. Gorden and Breach Science Publishers, New York
Sander B, Rasmussen B, Fredenslund A (1986) Calculation of vapour-liquid equilibria in nitric acid–water–nitrate salt systems using an extended UNIQUAC equation. Chem Eng Sci 41:1185–1195
Danesi PR, Orelandini F, Scibona G (1966) Determination of the stability constant of nitrate, chloride, and bromide complexes of Pu(IV). J Inorg Nucl Chem 28:1047–1054
Laxminarayanan T, Patil S, Sharma H (1964) Mechanism of extraction of Plutonium(IV) in organic solvents. J Inorg Nucl Chem 26:1001–1009
Berg J, Veirs DK, Vaughn R, Cisneros M, Smith C (1998) Plutonium(IV) mononitrate and dinitrate complex formation in acid solutions as a function of ionic strength. J Radioanal Nucl Chem 235:25–29
Veirs DK, Smith C, Berg J, Zwick B, Marsh SF, Allen P, Conradson S (1994) Characterization of nitrate complexes of P(IV) using absorption spectroscopy, 15 N NMR and EXAFS. J Alloy Compd 213(214):328–332
Greenwood NN, Earnshaw A (1984) Chemistry of the elements. Pergamon Press, Oxford
David FH, Vokmin V (2003) Thermodynamic properties of some tri- and tetravalent actinide aquo ions. New J Chem 27:1627–1632
Zemaitis JM, Clark DM, Rafal M, Scrivner NC (1986) Handbook of aqueous electrolyte thermodynamics. American Institute of Chemical Engineers, Design Institute for Physical Property Data, New York
Chaiko DJ, Tasker IR, Fredrickson DR, Difilippo AA, Smidt SM, Vandegrift GF (1993) Measurements of Al(NO3)3 activities in aqueous nitrate solutions. J Nucl Mater 201:184–189
Meissner HP, Kusik CL (1972) Activity coefficients of strong electrolytes in multicomponent aqueous solutions. AIChE J 18:294–298
Mikhailo VA (1968) Thermodynamics of mixed electrolyte solutions. Russ J Phys Chem 42:1414–1417
Pitzer KS (1973) Thermodynamics of electrolytes. I. Theoretical basis and general equations. J Chem Phys 77:268–277
Belair S, Labet A, Mariet C, Dannus P (2005) Modeling of the extraction of nitric acid and neodymium nitrate from aqueous solutions over a wide range of activities by CMPO. Solvent Extr Ion Exch 23:481–499
Pavicevic V, Ninkovic R, Todorovic M, Miladinovic J (1999) Osmotic and activity coefficients of yNaH2PO4 + (1−y) Na2SO4 (aq) at the temperature 298.15 K. Fluid Phase Equilib 164:275–284
Todorovic M, Ninkovic R (1997) Osmotic and activity coefficients of {xKNO3 + (1−x)MgSO4}(aq) at the temperature 298.15 K. J Chem Thermodyn 29:423–429
Charrin N, Moisy Ph, Blanc P (2000) Determination of fictive binary data for Plutonium(IV) nitrate. Radiochim Acta 88:25–31
Chan HS, Dill KA (1994) Solvation: effects of molecular size and shape. J Chem Phys 101:7007–7026
Liu Y, Watanasiri S (1996) Representation of liquid–liquid equilibrium of mixed-solvent electrolyte systems using the extended electrolyte NRTL model. Fluid Phase Equilib 116:193–200
Chen CC, Britt HI, Boston JF, Evans LB (1979) Extensions and applications of the Pitzer equation for vapor-liquid equilibrium of aqueous electrolyte systems with molecular solutes. AIChE J 25:820–831
Abrams DS, Prausnitz JM (1975) Statistical thermodynamics of liquid mixtures: a new expression for the excess Gibbs energy of partly or completely miscible systems. AIChE J 21:116–128
Mathias PM (2004) Correlation for the density of multicomponent aqueous electrolytes. Ind Eng Chem Res 43:6247–6252
Clarke SI, Mazzafro WJ (2005) In: Kirk R, Othmer D, Kroschwitz J, Howe-Grant M (eds) Kirk–Othmer encyclopedia of chemical technology, 4th edn. Wiley, New York
Ryan JL (1960) Species involved in the anion-exchange absorption of quadrivalent actinide nitrates. J Phys Chem 64:1375–1385
Slemmons A, Fitzpatrick J (2002) Separation of uranium and plutonium by various ion-exchange resins. Part I: time and nitric acid dependencies. Los Alamos National Laboratory Report LA-UR-02-4588
Ellis SRM, Thwaites JM (1957) Vapour–liquid equilibrium of nitric acid–water–sulphuric acid mixtures. J Appl Chem 7:152–160
Davis W, De Bruin HJ (1964) New activity coefficients of 0–100 per cent aqueous nitric acid. J Inorg Nucl Chem 26:1069–1083
Marsh SF, Jarvinen G, Kim JS, Nam J, Bartsch R (1997) New bifunctional anion-exchange resins for nuclear waste treatment. React Funct Polym 35:75–80