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A Chemical Reaction Calculation and a Semi-Empirical Model for the Dynamic Simulation of an Electrolytic Reduction of Spent Oxide Fuels  

Park, Byung-Heung (Korea Atomic Energy Research Institute)
Hur, Jin-Mok (Korea Atomic Energy Research Institute)
Lee, Han-Soo (Korea Atomic Energy Research Institute)
Publication Information
Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT) / v.8, no.1, 2010 , pp. 19-32 More about this Journal
Abstract
Electrolytic reduction technology is essential for the purpose of adopting pyroprocessing into spent oxide fuel as an alternative option in a back-end fuel cycle. Spent fuel consists of various metal oxides, and each metal oxide releases an oxygen element depending on its chemical characteristic during the electrolytic reduction process. In the present work, an electrolytic reduction behavior was estimated for voloxidized spent fuel based on the assumption that each metal-oxygen system is independent and behaves as an ideal solid solution. The electrolytic reduction was considered as a combination of a Li recovery and chemical reactions between the metal oxides such as uranium oxide and the produced Li metal. The calculated result revealed that most of the metal oxides were reduced by the process. It was evaluated that a reduced fraction of lanthanide oxides increased with a decreasing $Li_2O$ concentration. However, most of the lanthanides were expected to be stable in their oxide forms. In addition, a semi-empirical model for describing $U_3O_8$ electrolytic reduction behavior was proposed by considering Li diffusion and a chemical reaction between $U_3O_8$ and Li. Experimental data was used to determine model parameters and, then, the model was applied to calculate the reduction yield with time and to estimate the required time for a 99.9% reduction.
Keywords
Pyroprocessing; Spent Oxide Fuel; Electrolytic Reduction; Model; Simulation;
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Times Cited By KSCI : 3  (Citation Analysis)
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1 P. Kar and J.W. Evans, "A Shrinking Core Model for the Electro-deoxidation of Metal Oxides in Molten Halides Salts," Electrochim. Acta, 53, pp. 5260-5265 (2008).   DOI   ScienceOn
2 T. Usami, T. Kato, M. Kurata, T. Inoue, H. E. Sims, S. A. Beetharn, and J. A. Jenkins, "Lithhun Reduction of Americium Dioxide to Generate Americium Metal," J. Nucl. Mater., 304, pp. 50-55 (2002).   DOI   ScienceOn
3 T. Usami, M. Kurata, T. Inoue, H. E. Sims, S. A. Beetham, and J. A. Jenkins, "Pyrochemical Reduction of Uranium Dioxide and Plutonium Dioxide by Lithium Metal," J. Nucl. Mater., 300, pp. 15-26 (2002).   DOI   ScienceOn
4 G. Z. Chen, D.J. Fray, and T.W. Farthing, "Direct Electrochemical Reduction of Titanium Dioxide to Titanium in Molten Calcium Chloride," Nature, 407, pp. 361-362 (2000).   DOI   ScienceOn
5 B. H. Park and C.-S. Seo, "A Semi-empirical Model for the Air Oxidation Kinetics of $UO_{2}$," Korean J. Chem. Eng., 25(1), pp. 59-63 (2008).   DOI   ScienceOn
6 B. H. Park, S. M. Jeong, and C.-S. Seo, "Numerical Approach for the Voloxidation of an Advanced Spent Fuel Conditioning Process (ACP)," Proc. of Global 2007, Sep. 9-13, 2007, Boise, Idaho.
7 S. Herrmann, S. Li, and M. Simpson, "Electrolytic Reduction of Spent Light Water Reactor Fuel - Bench-Scale Experiment Results," J. Nucl. Sci. Technol., 44(3), pp. 361-367 (2007).   DOI   ScienceOn
8 M. Kurata, T. Inoue, J. Serg, M. Ougier, and J.P. Glatz, "Electro-chemical Reduction of MOX in LiCI," J. Nucl. Mater., 328, pp. 97-102 (2004).   DOI   ScienceOn
9 C. S. Seo, S. B. Park, B. H. Park, K. J. Jung, S. W. Park, and S. H. Kim, "Electrochemical Study on the Reduction Mechanism of Uranium Oxide in a LiCI-$Li_{2}O$ Molten Salt," J. Nucl. Sci. Technol., 43(5), pp. 587-595 (2006).   DOI   ScienceOn
10 Y. I. Chang, "The Integral Fast Reactor", Nucl. Technol., 88, pp. 129-138 (1989).
11 D. J. Fray, "Emerging Molten Salt Technologies for Metals Production," JOM, 53(10), pp. 26-31 (2001).
12 B. H. Park, S. B. Park, S. M. Jeong, C.-S. Seo, and S.-W. Park, "Electrolytic Reduction of Spent Oxide Fuel in a Molten LiCl-$Li_{2}$ System," J. Radioanal. Nucl. Chem., 270(3), pp. 575-583 (2006).   DOI   ScienceOn
13 박병흥, 강대승, 서중석, 박성원, "물질전달 모델 개발과 사용후핵연료 전기환원 공정에서의 세슘, 스트론튬, 바륨 및 산소 이온의 거동에 관한 작용," 방사성폐기물학회지, 3(2), pp. 85-93 (2005).   과학기술학회마을
14 B. H. Park, I. W. Lee, and C.-S. Seo, "Electrolytic Reduction Behavior of $U_{3}O_{3}$ in a Molten LiCI-$Li_{2}O$ Salt," Chem. Sci., 63, pp. 3485-3492 (2008).   DOI   ScienceOn
15 김정국, 김광락, 김인태, 안도희, 이한수, "파이로프로 세싱 발생 LiCl 염폐기물의 열발생," 방사성폐기물학회지, 7(2), pp. 73-78 (2009).   과학기술학회마을
16 Y. Deug, D. Wang, W. Xiao, X. Jin, X. Hu, and G. Z. Chen, "Electrochemistry at Conductor/Insulator/Electrolyte Three-Phase Interlines: A Thin Layer Model," J. Phys. Chern. B, 109(29), pp. 14043-14051 (2005).   DOI   ScienceOn
17 H. Assadi, "Phase-field Modelling of Electrodeoxidation in Molten Salt," Modelling Simul. Mater. Sci. Eng., 14, pp. 963-974 (2006).   DOI   ScienceOn
18 J.-M. Hur, C.-S. Seo, S.-S. Hong, D.-S. Kang, and S.W. Park, "Metalization of $U_{3}O_{8}$ via Catalytic Electrochemical Reduction with $Li_{2}O$ in LiCI Molten Salt,", React. Kinet. Catal. Lett., 80(2), pp. 217-222 (2003).
19 H. F. McFarlane and M. J. Lineberry, "The IFR Cycle Demonstration," Prog. Nucl. Energ., 31(1-2), pp. 155-173 (1997).   DOI   ScienceOn