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Equilibrium calculations for HyBRID decontamination of magnetite: Effect of raw amount of CuSO4 on Cu2O formation

  • Lee, Byung-Chul (Department of Chemical Engineering, Hannam University) ;
  • Kim, Seon-Byeong (Decommissioning Technology Research Division, Korea Atomic Energy Research Institute) ;
  • Moon, Jei-Kwon (Decommissioning Technology Research Division, Korea Atomic Energy Research Institute)
  • 투고 : 2019.12.18
  • 심사 : 2020.04.09
  • 발행 : 2020.11.25

초록

Calculations of chemical equilibrium for multicomponent aqueous systems of the HyBRID dissolution of magnetite were performed by using the HSC Chemistry. They were done by using a Pitzer-based aqueous solution model with the recipe of raw materials in experiments conducted at KAERI. The change in the amounts of species and ions and the pH values of the solution at equilibrium was observed as functions of temperature and raw amount of CuSO4. Precipitation of Cu2O occurred at a large amount of CuSO4 added to the solution, while no precipitation of Cu(OH)2 was found at any amounts of CuSO4. The E-pH diagrams for Cu were constructed at various Cu concentrations to provide the effect of the Cu concentration on the pH values at boundaries where the coexistence of Cu+ ion and Cu2O solid occurred. To prevent Cu+ ions from being precipitated to Cu2O, the raw amount of CuSO4 should be adjusted so that the pH value of the solution from the equilibrium calculation is less than that from the E-pH diagram. We provided guidelines for the raw amount of CuSO4 and the pH value of the solution, which prevent the formation of Cu2O precipitates in the HyBRID dissolution experiments for magnetite.

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참고문헌

  1. J.K. Moon, S.B. Kim, W.K. Choi, B.S. Choi, D.Y. Chung, B.K. Seo, The status and prospect of decommissioning technology development at KAERI, J. Nucl. Fuel Cycle Waste Technol. 17 (2019) 139-165. https://doi.org/10.7733/jnfcwt.2019.17.2.139
  2. Technical Report Series No, 395, State of the Art Technology for Decontamination and Dismantling of Nuclear Facilities, IAEA, Vienna, 1999.
  3. Technical Report Series No, 386, Decommissioning of Nuclear Facilities Other than Reactors, IAEA, Vienna, 1998.
  4. H.J. Won, W.S. Lee, C.H. Jung, S.Y. Park, W.K. Choi, J.K. Moon, A feasibility study on the decontamination of type 304 stainless steel by $N_2H_4$ base solution, Asian J. Chem. 26 (2014) 1327-1330. https://doi.org/10.14233/ajchem.2014.17221
  5. J.Y. Jung, S.Y. Park, H.J. Won, S.B. Kim, W.K. Choi, J.K. Moon, S.J. Park, Corrosion properties of inconel-600 and 304 stainless steel in new oxidative and reductive decontamination reagent, Met. Mater. Int. 21 (2015) 678-685. https://doi.org/10.1007/s12540-015-4572-x
  6. W.K. Choi, Development of Advanced Decontamination Technology for Nuclear Facilities, KAERI, 2017. Report No. 2012M2A8A5025655.
  7. W.K. Choi, H.J. Won, S.Y. Park, S.B. Kim, J.Y. Jung, J.K. Moon, Chemical decommissioning of a primary coolant system using hydrazine-based solutions, in: Waste Management Conference, Proceedings, Paper No 15215, Phoenix, Arizona, USA, March 15-19, 2015.
  8. H.J. Won, W.S. Lee, C.H. Jung, S.Y. Park, W.K. Choi, J.K. Moon, Dissolution of $Fe_3O_4$ by the $N_2H_4$ base solution, in: 7th International Conference on Multifunctional Materials and Applications, Proceedings, Huainan, China, Nov., vols. 22-23, 2013.
  9. B.-C. Lee, S.-B. Kim, J.-K. Moon, S.-Y. Park, Evaluation of reaction spontaneity for acidic and reductive dissolutions of corrosion metal oxides using HyBRID chemical decontamination, J. Radioanal. Nucl. Chem. 323 (2020) 91-103. https://doi.org/10.1007/s10967-019-06962-3
  10. S.-B. Kim, S.-Y. Park, W.-K. Choi, H.-J. Won, J.-S. Park, B.-K. Seo, Magnetite dissolution by copper catalyzed reductive decontamination, J. Nucl. Fuel Cycle Waste Technol. 16 (2018) 421-429. https://doi.org/10.7733/jnfcwt.2018.16.4.421
  11. K.S. Pitzer, Thermodynamics of electrolytes. I. Theoretical basis and general equations, J. Phys. Chem. 77 (1973) 268-277. https://doi.org/10.1021/j100621a026
  12. C.E. Harvie, J.H. Weare, The prediction of mineral solubilities in natural waters: the Na-K-Mg-Ca-Cl-$SO_4-H_2O$ system from zero to high concentration at $25^{\circ}C$, Geochem. Cosmochim. Acta 44 (1980) 981-997. https://doi.org/10.1016/0016-7037(80)90287-2
  13. C.E. Harvie, N. Moller, J.H. Weare, The prediction of mineral solubilities in natural waters: the Na-K-Mg-Ca-H-Cl-$SO_4$-OH-$HCO_3-CO_3-CO_2-H_2O$ system to high ionic strengths at $25^{\circ}C$, Geochem. Cosmochim. Acta 48 (1984) 723-751. https://doi.org/10.1016/0016-7037(84)90098-X
  14. K.S. Pitzer, Thermodynamics, third ed., McGraw-Hill, 1995.
  15. K.S. Pitzer, Activity Coefficients in Electrolyte Solutions, CRC Press, 1979.
  16. J.M. Prausnitz, R.N. Lichtenthaler, E. Gomes de Azevedo, Molecular Thermodynamics of Fluid- Phase Equilibria, third ed., Prentice-Hall, 1999.
  17. J.F. Zemaitis Jr., D.M. Clark, M. Rafal, N.C. Scrivner, Handbook of Aqueous Electrolyte Thermodynamics, Wiley-Interscience, 1986.
  18. HSC Chemistry software. www.outotec.com.
  19. H. Haung, Construction of Eh-pH and other stability diagrams of uranium in a multicomponent system with a microcomputer-I. Domains of predominance diagrams, Canadian Metallurgical Quarterly 28 (1989) 225-239. https://doi.org/10.1179/cmq.1989.28.3.225