Uranyl nitrate hexahydrate solubility in nitric acid and its crystallization selectivity in the presence of nitrate salts

被引：14

作者：

Burns, Jonathan D. ^{[1
]}

Moyer, Bruce A. ^{[2
]}

机构：

[1] Texas A&M Univ, Nucl Sci Secur & Policy Inst, College Stn, TX 77845 USA

[2] Oak Ridge Natl Lab, Chem Sci Div, POB 2008, Oak Ridge, TN 37831 USA

来源：

JOURNAL OF CLEANER PRODUCTION | 2018年 / 172卷

关键词：

Uranyl nitrate solubility; Actinide co-crystallization; Crystallization selectivity; Separation; Actinide; NUCLEAR-POWER; SEPARATIONS; AMERICIUM; OXIDATION; EXTRACTION; ACTINIDES; BEHAVIOR;

D O I：

10.1016/j.jclepro.2017.10.258

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

The solubility of uranyl nitrate hexahydrate was determined as a function of nitric acid concentration and temperature, and the crystallization yield was calculated. Results showed an increase in crystal formation at lower initial nitric acid concentrations upon cooling a saturated solution of U(VI) from 50 degrees C to 2 degrees C, with over 70% recovery of U(VI) mass at all nitric acid concentrations and nearly quantitative recovery starting at 4 M HNO3. A direct correlation between the change in mother liquor volume percent and U mass removal percent was observed. By reducing the cooling rate from roughly 4.0 C/min to 0.22 C/min, the separation factor was increased from 3.88 to 15.7 to greater than 81 for the separation of U(VI) from Sr, Cs, and Nd. At the slower cooling rate, the separation factors were measured as a function of acidity for 2.0-4.3 M HNO3, showing a decrease in selectivity with a decrease in the acidity. There was also no indication that tetravalent metal double-salt precipitation occurred with either Zr4+ or Ce4+. These results indicate that a high-yield, high purity hexavalent actinide crystallization scheme may offer attractive benefits for nuclear-fuel recycle in that only a single very simple and well-understood technology is employed, and the use of organic compounds and solvents is avoided. (C) 2017 Elsevier Ltd. All rights reserved.

引用

页码：867 / 871

页数：5

共 29 条

[11] Electrochemical oxidation of 243Am(III) in nitric acid by a terpyridyl-derivatized electrode [J].

Dares, Christopher J. ;

Lapides, Alexander M. ;

Mincher, Bruce J. ;

Meyer, Thomas J. .

SCIENCE, 2015, 350 (6261) :652-655

[12] Generating the Option of a Two-Stage Nuclear Renaissance [J].

Grimes, Robin W. ;

Nuttall, William J. .

SCIENCE, 2010, 329 (5993) :799-803

[13]

Haynes W. M., 2016, CRC HDB CHEM PHYS, DOI 10.1201/9781315380476

[14] Prevented Mortality and Greenhouse Gas Emissions from Historical and Projected Nuclear Power [J].

Kharecha, Pushker A. ;

Hansen, James E. .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (09) :4889-4895

[15]

Miguirditchian M., 2007, In GANEX: Adaptation of the DIAMEX-SANEX process for the group actinide separation, P550

[16]

Mincher B.J., 2015, J RADIOANAL NUCL CHE

[17] Tributylphosphate extraction behavior of bismuthate-oxidized americium [J].

Mincher, Bruce J. ;

Martin, Leigh R. ;

Schmitt, Nicholas C. .

INORGANIC CHEMISTRY, 2008, 47 (15) :6984-6989

[18] Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution [J].

Mincher, Bruce J. ;

Schmitt, Nicholas C. ;

Schuetz, Brian K. ;

Shehee, Thomas C. ;

Hobbs, David T. .

RSC ADVANCES, 2015, 5 (34) :27205-27210

[19] DIAMYLAMYLPHOSPHONATE SOLVENT EXTRACTION OF AM(VI) FROM NUCLEAR FUEL RAFFINATE SIMULANT SOLUTION [J].

Mincher, Bruce J. ;

Martin, Leigh R. ;

Schmitt, Nicholas C. .

SOLVENT EXTRACTION AND ION EXCHANGE, 2012, 30 (05) :445-456

[20]

Moyer B.A., 2015, REPROCESSING RECYCLI, P289, DOI DOI 10.1016/B978-1-78242-212-9.00011-3

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