TBP에 의한 모의방사성 폐액 내 Re, Np 및 잔존 U의 선택적 분리

이일희; 김수호; 임재관; 김광욱; 유재형; Eil Hee Lee; Soo Ho Kim; Jae Gwan Lim; Kwang Wook Kim; Jae-Hyung Yoo

HWAHAK KONGHAK, Vol.39, No.1, 36-42, February, 2001

A Selective-Separation of Re, Np and Residual U from the Simulated Radwaste Solution Containing the Oxidant of Np by Solvent Extraction with Tributyl Phosphate

이일희 ^†, 김수호, 임재관, 김광욱 , 유재형

한국원자력연구소

Eil Hee Lee^†, Soo Ho Kim, Jae Gwan Lim, Kwang Wook Kim , and Jae-Hyung Yoo

Korea Atomic Energy Research Institute, Korea

E-mail:

초록

Np의 산화제로 1g/L NH₄VO₃ 함유된 10 성분계의 모의방사성 폐액으로부터 Re, Np 및 잔존 U만을 선택적으로 분리하기 위하여 TBP에 의한 이들의 공추출과 역추출 거동 규명 및 이의 조업조건을 고찰하였다. Re, Np, U의 공추출 조건으로는 TBP의 농도를 증가시키는 것보다 O/A 비를 2정도로 증가시키는 것이 효과적이다. 그리고 Re, Np, U 등이 공추출된 유기상으로부터 NBA에 의해 Np만을 선택적으로 환원 역추출할 수 있으며, 조건으로는 Np이 67% 역추출되는 NBA=1.04M, O/A=1이 적당하다. 이때 Re이 70% 정도 Np과 같이 공역추출되므로 Np의 분리에 앞서 Re을 미리 제거시켜야 한다. 한편 Re의 선택적 역추출은 O/A 비 변화를 통한 Np의 공역추출 감소가 요구되고 있으며, Re 및 Np이 각각 80%, 6%로 역추출되는 5M 질산, O/A=4가 적당하다. 반면에 U의 선택적 역추출은 U의 분리에 앞서 Re과 Np을 미리 제거시켜야 하며, 0.01M 질산, O/A=7에서 약 76%의 U이 역추출되었다.

For the selective separation of Re, Np and residual U from the 10 components simulated radwaste solution containing the NH4VO3 of 1 g/L as an oxidant of Np, the behavior of co-extraction by tributyl phosphate/n-dodecane and stripping of Re, Np, U and their operation conditions were evaluated. Co-extraction of Re, Np and U was more effective increase of O/A ratio than with increase of TBP concentration. Co-extraction yields of their elements were 28.6%, 93.8% and 96.2% at O/A=2, respectively. It was found that Np was effectively stripped by reduction with a NBA (normal butyraldehyde) from the loaded organic phase. At 1.04 M NBA and O/A=1, Np and Re was co-stripped about 67% and 70%, respectively. So, Re must be removed before separation of Np. Stripping of Re, however, was needed the decrease of the co-stripping yields of Np with change of O/A ratio. At 5 M HNO3 and O/A=4, Np and Re was co-stripped about 80% and 6%, respectively. On the other hand, Re and Np must be removed before separation of U. U was stripped about 76% at 0.01 M HNO3 and O/A=7.

Keywords:Rhenium;Neptunium;Uranium;Oxidation/Reduction;Tributyl Phosphate

[References]

OECD Final Report: Status and Assessment Report on Actinide and Fission Product Partitioning and transmutation, NEA/PTS/DOC(98)4 (1998)
Takayanagi M, Fujine S, Muraoka S, Kubota M, Adachi T, Miyoshi Y, Banba T, Ohnuki T, Sato T, Safety Research and Development of Base Technology on Nuclear Fuel Cycle, JAERI-Conf 99-004 (1999)
ICRP report: Limits for Intake of Radionuclides by Workers, ICRP Publication, Part I(1978), Part II(1980), Part III(1981)
Kondo Y, Takitsuka T, Technology Assessment of Partitioning Process, JAERI-M 94-067 (1994)
Fabienne W, Oxydo-Reduction du Np dans les melanges phosphate tributylique/ dodecane, CEA-R-5478 (1989)
Lelievre D, Boussier H, Grouiller JP, Bush RP, Perspectives and Cost of Partitioning and Transmutation of Long-lived Radio-nuclides, EUR-17485 (1996)
Kolarik Z, Dressler P, Solv. Extr. Ion Exch., 7(4), 625 (1989)
Lee EH, Kim KW, Lim JG, Kwon SG, Yoo JH, J. Korean Ind. Eng. Chem., 9(2), 232 (1998)
Benedit M, Pigford TH, Levi HW, "Nuclear Chemical Engineering," 2nd Edt., McGraw-Hill Book Company (1981)
Tanaka C, Nemoto S, Tsubota T, Hoshino T, "Analytical chemistry of Np," PNCT-841-71-35 (1971)
Lee EH, Kim KW, Chung DY, Kwon SG, Yoo JH, HWAHAK KONGHAK, 37(3), 439 (1999)
Lee EH, Lim JK, Kim KW, Kwon SG, Yoo JH, Park HS, HWAHAK KONGHAK, 37(6), 897 (1999)
Morita Y, Kubota M, Recovery of Neptunium, JAERI-M-84-043 (1984)
Kondo Y, Takitsuka T, Technology Assessment of Partitioning Process, JAERI-M 94-067 (1994)
Apostolidis C, Glatz JP, Molinet R, Recovery of MA from Irradiated SUPERFACT Fuels, Global 1995, Versailles, France, 2, 1027 (1995)
Pruett DJ, The Solvent Extraction of Heptavalent Technetium and Rhenium by Tributyl Phosphate, ORNL/TM-8668 (1984)
Schulz WW, Burger LL, Navratil JD, Bender KP, Science and Technology of TBP, CRC Press, Ins., Florida, USA (1990)
Uchiyama G, Hotoku S, Fujine S, Maeda M, Separation of Np, Pu and U by using Butyraldehydes as Reductants in Reprocessing, JAERI-M 93-198 (1993)
Bard AJ, Parsons R, Jordan J, "Standard Potentials in Aqueous Solution," Marcell Dekker, Inc. New York, USA (1985)

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[1] OECD Final Report: Status and Assessment Report on Actinide and Fission Product Partitioning and transmutation, NEA/PTS/DOC(98)4 (1998)

[2] Takayanagi M, Fujine S, Muraoka S, Kubota M, Adachi T, Miyoshi Y, Banba T, Ohnuki T, Sato T, Safety Research and Development of Base Technology on Nuclear Fuel Cycle, JAERI-Conf 99-004 (1999)

[3] ICRP report: Limits for Intake of Radionuclides by Workers, ICRP Publication, Part I(1978), Part II(1980), Part III(1981)

[4] Kondo Y, Takitsuka T, Technology Assessment of Partitioning Process, JAERI-M 94-067 (1994)

[5] Fabienne W, Oxydo-Reduction du Np dans les melanges phosphate tributylique/ dodecane, CEA-R-5478 (1989)

[6] Lelievre D, Boussier H, Grouiller JP, Bush RP, Perspectives and Cost of Partitioning and Transmutation of Long-lived Radio-nuclides, EUR-17485 (1996)

[7] Kolarik Z, Dressler P, Solv. Extr. Ion Exch., 7(4), 625 (1989)

[8] Lee EH, Kim KW, Lim JG, Kwon SG, Yoo JH, J. Korean Ind. Eng. Chem., 9(2), 232 (1998)

[9] Benedit M, Pigford TH, Levi HW, "Nuclear Chemical Engineering," 2nd Edt., McGraw-Hill Book Company (1981)

[10] Tanaka C, Nemoto S, Tsubota T, Hoshino T, "Analytical chemistry of Np," PNCT-841-71-35 (1971)

[11] Lee EH, Kim KW, Chung DY, Kwon SG, Yoo JH, HWAHAK KONGHAK, 37(3), 439 (1999)

[12] Lee EH, Lim JK, Kim KW, Kwon SG, Yoo JH, Park HS, HWAHAK KONGHAK, 37(6), 897 (1999)

[13] Morita Y, Kubota M, Recovery of Neptunium, JAERI-M-84-043 (1984)

[14] Kondo Y, Takitsuka T, Technology Assessment of Partitioning Process, JAERI-M 94-067 (1994)

[15] Apostolidis C, Glatz JP, Molinet R, Recovery of MA from Irradiated SUPERFACT Fuels, Global 1995, Versailles, France, 2, 1027 (1995)

[16] Pruett DJ, The Solvent Extraction of Heptavalent Technetium and Rhenium by Tributyl Phosphate, ORNL/TM-8668 (1984)

[17] Schulz WW, Burger LL, Navratil JD, Bender KP, Science and Technology of TBP, CRC Press, Ins., Florida, USA (1990)

[18] Uchiyama G, Hotoku S, Fujine S, Maeda M, Separation of Np, Pu and U by using Butyraldehydes as Reductants in Reprocessing, JAERI-M 93-198 (1993)

[19] Bard AJ, Parsons R, Jordan J, "Standard Potentials in Aqueous Solution," Marcell Dekker, Inc. New York, USA (1985)