모의 방사성용액에서 란탄족과 악티늄족원소의 옥살산침전

정동용; 김응호; 이일희; 유재형; 박현수

Journal of the Korean Industrial and Engineering Chemistry, Vol.10, No.7, 996-1002, November, 1999

Export Citation

모의 방사성용액에서 란탄족과 악티늄족원소의 옥살산침전

Oxalate Precipitation of Lanthanide and Actinide in a Simulated Radioactive Liquid Waste

정동용, 김응호, 이일희, 유재형, 박현수

초록

알칼리 및 알칼리토금속(Cs, Rb, Ba, Sr), 전이금속(Zr, Fe, Mo, Ni, Pd, Rh), 란탄족(La, Y, Nd, Ce, Eu) 및 악티늄족(Np, Am) 등 17개 원소로 구성된 질산매질의 모의 방사성용액에서 옥살산에 의한 란탄족과 악티늄족 원소의 공침전 연구를 수행하였다. 옥살산 농도 0.5 M에서 질산농도으 영향과 아스코빅산 첨가에 따른 원소들의 침전율이 조사되었다. 각 원소들의 침전율은 질산농도에 따라 약간 감소하였으나 란탄족과 악티늄족은 99% 이상 침전외었다. 옥살산 침전시 아스코빅산이 척가되는 경우 Pd이 금속으로 환원 침전되었고, 이때 Mo, Fe, Ni, Ba의 경우는 침전율이 약 10~20% 감소하는 것으로 나타났으나, 기타 원소들에 대해서는 영향이 나타나지 않았다. Pd(II) 이온은 질산농도 1.0 M 미만의 모의용액에서 아스코빅산 첨가시 Pd 금속으로의 환원침전이 일어났으며, 아스코빅산 농도가 0.01~0.02 M 부근에서 가장 크게 나타났다. 하이드라진이 아스코빅산과 같이 첨가될 때 Pd의 환원침전을 억제하는 것으로 나타났다.

The oxalate precipitation of lanthanide and actinide by oxalic acid was investigated in the simulated radioactive liquid waste, which was conposed of 17 elements of alkali, alkaline earth(Cs, Rb, Ba, Sr), transition metal(Zr, Fe, Mo, Ni, Pd, Rh), lanthanide(La, Y, Nd, Ce, Eu)and actinide(Np, Am) in nitrc acid solution. The effect of concentrations of nitric acid and ascorbic acid on the precipitation yield of each element in the simulated solution was examined at 0.5 M oxalic acid concentration. The precipitation yields of the elements were usually decreased with nitric acid concentration, nevertheless, the precipitation yields of lanthanide and actinide were more than 99%. Palladium was precipitated due to the reduction of Pd(II) into Pd metal by the addition of ascorbic acid in the oxalate precipitation and then, the precipitation yields of Mo, Fe, Ni, Ba decreased by 10~20% with concentration of ascorbic acid. The reductive precipitation of Pd(II) into Pd metal by the addition of ascorbic acid into the simulated radwaste occurred at below 1 M nitric acid concentration and its yield showed maximum at the ascorbic acid concentration of 0.01~0.02 M. The hydrazine suppressed the reductive precipitation of Pd by the ascorbic acid.

Keywords:oxalate precipitation;ascorbic acid;hydrazine;actinide;lanthanide

[References]

IAEA Technical Reports Series No 214, "Evaluation of Actinide Partitioning and Transmutation," IAEA, VIENNA (1982)
유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1322/94 (1993)
정동용, 김응호, 김원호, 신영준, 유재형, '95 춘계학술발표회 논문집 (II), 한국원자력학회, 793 (1995)
Kubota M, Yamaguchi I, Okada K, Morita Y, Nakamura H, "Development of Partitioning Test with Nuclear Fuel Reprocessing Waste Prepared at PNC - part 1," JAERI-M83-011 (1983)
Yamaguchi I, Kubota M, Okade K, Morita Y, Nakamura H, "Development of Partitioning Method: Patitioning Test with Nuclear Fuel Reprocessing Wastes Prepared at PNC - part 2 -," JAERI-M85-070 (1980)
Fujime S, Usuda S, Morita Y, Yoshida Z, Suzuki Y, Furuta T, Tome T, Ohta K, Nishimura K, Hasegawa S, "Conceptual Design of Backend Technology R&D Facility for TRU Recycle in the Future Fuel Cycle System," JAERI-M93-211 (1993)
Posey JC, "Process for the Recovery of Cm-244 from Nuclear Waste," ORNL-5687 (1980)
Miyashio H, Kubota M, "Development of Partitioning Method: Fundamental Study on Oxalate Precipitation Method," JAERI-M86-014 (1986)
IAEA Technical Reports Series No. 137, "Chemical Precipitation Process for the Treatment of Aqueous Radioactive Waste," IAEA, Vienna (1992)
Tedder DW, Blomeke JO, "Actinide Partitioning and Transmutation Program Progress Report for Period April 1 to June 30, 1977," ORNL/TM-6056 (1977)
Rankin DT, Burney GA, Smith PK, Sission RD, Ceram. Bull., 56, 478 (1977)
Kobayashi T, Morita Y, Kubota M, "Development of Partitioning Method: Method of Precipitating Transuranium Elements with Oxalic Acid," JAERI-M88-026 (1988)
Kobayachi T, Shirahashi K, Kubota M, "Development of Partitioning Method: Precipitation Behavior of Other Elements in Separating the Transuranic Elements Group with Oxalic Acid," JAERI-M89-168 (1989)
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International Commission on Radiation Protection, Limits for Intake of Radionuclides by Workers, ICRP Publication, Part II, International Atomic Energy Agency (1980)
International Commission on Radiation Protection, Limits for Intake of Radionuclides by Workers, ICRP Publication, Part III, International Atomic Energy Agency (1981)
유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1467/95 (1994)
Kim EH, Shin YJ, Kim WH, Chung DY, Kim SS, Yoo JH, Choi CS, Korean J. Chem. Eng., 12(5), 557 (1995)
Chung DY, Kim EH, Shin YJ, Yoo JH, Kim JD, J. Korean Ind. Eng. Chem., 6(4), 589 (1995)
Chung DY, Kim EH, Shin YJ, Yoo JH, Choi CS, Kim JD, J. Radioanal. Nucl. Chem. Lett., 201, 495 (1995)
Chung DY, Kim EH, Shin YJ, Yoo JH, Kim JD, HWAHAK KONGHAK, 34(4), 451 (1996)
Kim EH, Chung DY, Kim WH, Shin YJ, Lee EH, Yoo JH, Choi CS, J. Nucl. Sci. Technol., 34, 283 (1997)
이일희, 유재형, 정동용, 군분리공정 평가, KAERI/TR-960/98 (1998)
유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1632/95 (1995)
Chung DY, Kim EH, Lee EH, Yoo JH, J. Ind. Eng. Chem., 4(4), 277 (1998)
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Kirk RE, Othmer DF, Encyclopedia of Chemical Technology, 3rd ed., Wiley, New York (1980)
Rickman RA, Sorensen RL, Watkins KO, Davies G, Inorg. Chem., 16, 1570 (1977)
Bard AJ, Parsons R, Jordon J, Standard Potentials in Aqueous Solution, Marcel Dekker, Inc., New York (1985)
Creutz C, Inorg. Chem., 20, 4449 (1981)

[1] IAEA Technical Reports Series No 214, "Evaluation of Actinide Partitioning and Transmutation," IAEA, VIENNA (1982)

[2] 유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1322/94 (1993)

[3] 정동용, 김응호, 김원호, 신영준, 유재형, '95 춘계학술발표회 논문집 (II), 한국원자력학회, 793 (1995)

[4] Kubota M, Yamaguchi I, Okada K, Morita Y, Nakamura H, "Development of Partitioning Test with Nuclear Fuel Reprocessing Waste Prepared at PNC - part 1," JAERI-M83-011 (1983)

[5] Yamaguchi I, Kubota M, Okade K, Morita Y, Nakamura H, "Development of Partitioning Method: Patitioning Test with Nuclear Fuel Reprocessing Wastes Prepared at PNC - part 2 -," JAERI-M85-070 (1980)

[6] Fujime S, Usuda S, Morita Y, Yoshida Z, Suzuki Y, Furuta T, Tome T, Ohta K, Nishimura K, Hasegawa S, "Conceptual Design of Backend Technology R&D Facility for TRU Recycle in the Future Fuel Cycle System," JAERI-M93-211 (1993)

[7] Posey JC, "Process for the Recovery of Cm-244 from Nuclear Waste," ORNL-5687 (1980)

[8] Miyashio H, Kubota M, "Development of Partitioning Method: Fundamental Study on Oxalate Precipitation Method," JAERI-M86-014 (1986)

[9] IAEA Technical Reports Series No. 137, "Chemical Precipitation Process for the Treatment of Aqueous Radioactive Waste," IAEA, Vienna (1992)

[10] Tedder DW, Blomeke JO, "Actinide Partitioning and Transmutation Program Progress Report for Period April 1 to June 30, 1977," ORNL/TM-6056 (1977)

[11] Rankin DT, Burney GA, Smith PK, Sission RD, Ceram. Bull., 56, 478 (1977)

[12] Kobayashi T, Morita Y, Kubota M, "Development of Partitioning Method: Method of Precipitating Transuranium Elements with Oxalic Acid," JAERI-M88-026 (1988)

[13] Kobayachi T, Shirahashi K, Kubota M, "Development of Partitioning Method: Precipitation Behavior of Other Elements in Separating the Transuranic Elements Group with Oxalic Acid," JAERI-M89-168 (1989)

[14] International Commission on Radiation Protection, Limits for Intake of Radionuclides by Workers, ICRP Publication, Part I, International Atomic Energy Agency (1978)

[15] International Commission on Radiation Protection, Limits for Intake of Radionuclides by Workers, ICRP Publication, Part II, International Atomic Energy Agency (1980)

[16] International Commission on Radiation Protection, Limits for Intake of Radionuclides by Workers, ICRP Publication, Part III, International Atomic Energy Agency (1981)

[17] 유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1467/95 (1994)

[18] Kim EH, Shin YJ, Kim WH, Chung DY, Kim SS, Yoo JH, Choi CS, Korean J. Chem. Eng., 12(5), 557 (1995)

[19] Chung DY, Kim EH, Shin YJ, Yoo JH, Kim JD, J. Korean Ind. Eng. Chem., 6(4), 589 (1995)

[20] Chung DY, Kim EH, Shin YJ, Yoo JH, Choi CS, Kim JD, J. Radioanal. Nucl. Chem. Lett., 201, 495 (1995)

[21] Chung DY, Kim EH, Shin YJ, Yoo JH, Kim JD, HWAHAK KONGHAK, 34(4), 451 (1996)

[22] Kim EH, Chung DY, Kim WH, Shin YJ, Lee EH, Yoo JH, Choi CS, J. Nucl. Sci. Technol., 34, 283 (1997)

[23] 이일희, 유재형, 정동용, 군분리공정 평가, KAERI/TR-960/98 (1998)

[24] 유재형, 이일희, 정동용, 장수명핵종 소멸처리 기술개발, KAERI/RR-1632/95 (1995)

[25] Chung DY, Kim EH, Lee EH, Yoo JH, J. Ind. Eng. Chem., 4(4), 277 (1998)

[26] Keller C, The Chemistry of the Transuranium Elements, Verlag Chemie GmbH, Weinheim/Bergstr (1971)

[27] Burney GA, Harbour RM, Radiochemistry of Neptunium, NAS-NS-3060 (1974)

[28] Davies MB, Polyhedron, 11, 285 (1992)

[29] Kirk RE, Othmer DF, Encyclopedia of Chemical Technology, 3rd ed., Wiley, New York (1980)

[30] Rickman RA, Sorensen RL, Watkins KO, Davies G, Inorg. Chem., 16, 1570 (1977)

[31] Bard AJ, Parsons R, Jordon J, Standard Potentials in Aqueous Solution, Marcel Dekker, Inc., New York (1985)

[32] Creutz C, Inorg. Chem., 20, 4449 (1981)