Journal of Nuclear Science, Engineering and Technology (JONSAT)
In cooperation with the Iranian Nuclear Society

Qualitative and quantitative determination of technetium-99 in the concentrated waste of Bushehr nuclear power plant

Document Type : Research Paper

Authors

R. Yavari 1
K. Saberian 1
A. Maleki Farsani 2
B. Salimi 1
B. Soleimanzade 2
A. Heydari 2
M. Tabasi 1

1 Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, AEOI, P.O.Box: 11365-8486, Tehran - Iran

2 Iran Radioactive Waste Company, AEOI, Postal Code: 1437643531, Tehran - Iran

https://doi.org/10.24200/nst.2024.1649
Abstract
Technetium-99 in nuclear waste as one of the toxic and hazardous radioactive pollutants should be quantitatively and qualitatively identified before final disposal. In the present research work, Technetium -99 in the aqueous phase of the concentrated waste of Bushehr nuclear power plant was qualified and quantified. To achieve this goal, Cesium-134 and 137 were firstly separated using potassium cobalt hexacyanoferrate(II) adsorbent. Then, tritium was removed using thermal treatment at 60˚C, and finally technetium-99 in this media was purified by removing beta emitter radioisotopes such as cobalt- 60, iron-55, and nickel-63 using precipitation process with iron(III) hydroxide. The samples were qualitatively and quantitatively evaluated using gamma spectrometry and liquid scintillation counter instruments. The results showed that purified Technetium-99 has a high radiochemical purity and other radioisotopes were removed from the media with an efficiency of about 100%. Also, the beta spectrum of the sample was in complete accordance with the beta spectrum of the standard samples. The total yield of the proposed processes using the increase of Technetium-99m tracer to the original sample was equivalent to 80.69%. Taking into account the 93% efficiency of the liquid scintillation counter and the processes yield (80.69%), the specific activity of Technetium-99 was calculated as 10554.13 Bq.L-1.

Highlights

  1. Hou X. Liquid Scintillation Counting for Determination of Radionuclides in Environmental and Nuclear Application. Journal of Radioanalytical and Nuclear Chemistry. 2018;318:1597–1628.

 

  1. Shi K.L, Hou X.L, Roos P, Wu W.S. Determination of Technetium-99 in Environmental Samples: A Review. Analtical Chimica Acta. Analtical Chim Acta. 2011;709:1–20.

 

  1. Rozas S, López J, Idoeta R, Herranz M. Selectivity Analysis of 99Tc Determination by LSC in the Field of Nuclear Decommissioning. Journal of Radioanalytical and Nuclear Chemistry. 2022;331:3335–3341.

 

  1. Butterworth J.C, Livens F.R, Makinson P.R. Development of a Method for the Determination of Low Levels of Technetium-99. The Science of the Total Environment. 1995;173/174:293-300.

 

  1. Reis A.S, Temba E.S.C, Kastner G.F, Monteiro R.P.G. Isolation and Activity Determination of 99Tc in Nuclear Waste by Liquid Scintillation Counting. 2011 International Nuclear Atlantic Conference- INAC. 2011.

 

  1. Chao J.H, Tseng C.L, Lee C.J. Sequential Extraction Separation for Determination of Technetium-99 in Radwastes by ICP-MS. Journal of Radioanalytical and Nuclear Chemistry. 2002:251(1);105-112.

 

  1. Shia K, Houa X, Roosa P, Wub W. Determination of Technetium-99 in Environmental Samples: A review. Analytica Chimica Acta. 2012:709;1–20.

 

  1. Momoshima N, Sayad M, Takashima Y. Analytical Procedure for Technetium-99 in Seawater by ICP-MS. Radiochimca Acta. 1993;63:73–78.

 

  1. Ikaheimonen T.K, Vartti V.P, Ilus E, Mattila J. Technetium-99 in Fucus and Seawater Samples in the Finnish Coastal Area of the Baltic Sea. Journal of Radioanalytical and Nuclear Chemistry. 1999:252:309–313.

 

  1. Goken G.L, Bruening R.L, Krakowiak K.E, Izatt R.M. Metalion Separations Using Superlig or Analig Materials Encased in Empore Cartriges and Disks. ACS Symposium Series 716, American Chemical Society, Washington, DC. 1999;251–529.

 

  1. Izatt S.R, Bruening R.L, Krakowiak K.E, Izatt R.M. The Selective Separation of Anions and Cations in Nuclear Waste Using Commercially Available Molecular Recognition Technology Products. Proceedings of WM’03 Conference, Tuscon. 2003.

 

  1. Remenec B, Dulanska S, Paucova V, Matel L. Determination of 99Tc in Evaporator Concentrates Using Solid Phase Extraction Techniques. Journal of Radioanalytical and Nuclear Chemistry. 2011;290:403–407.

 

  1. Uchida S, Tagami K. Separation and Concentration of Technetium Using A Tc-Selective Extraction Chromatographic Resin. Journal of Radioanalytical and Nuclear Chemistry. 1997;221:35–39.

 

  1. Dixon P, Curtis D.B, Musgrave J, Roensch F, Roach J, Rokop D. Analysis of Naturally Produced Technetium and Plutonium in Geologic Materials. Analalytical Chemistry. 1997;69:1692–1699.

 

  1. Prout W.E. Russell E.R, Groh H.J. Ion Exchange Absorption of Cesium by Potassium Hexacyanocobalt (II) Ferrate (II). Journal of Inorganic and Nuclear Chemistry. 1965;27:473-479.

 

  1. Ru Y, Zheng S, Xue H, Pang H. Potassium Cobalt Hexacyanoferrate Nanocubic Assemblies for High-Performance Aqueous Aluminum Ion Batteries. Chemical Engineering Journal. 2020;382:122853.

 

  1. Hou X.L. Radiochemical Determination of 41Ca in Reactor Concrete for Decommissioning. Radiochimca Acta. 2005;93:611–617.

 

  1. Hou X.L. Radiochemical Analysis of Radionuclides Difficult to Measure or Waste Characterization in Decommissioning of Nuclear Facilities. Journal of Radioanalytical and Nuclear Chemistry. 2007;273:43–48.

 

  1. Hou X.L, Frøsig L, Nielsen S.P. Determination of 36Cl in Nuclear Waste from Reactor Decommissioning. Analalytical Chemistry. 2007;79:3126–3134.

 

  1. Hou X.L, Ostergaard L.F, Nielsen S.P. Determination of 63Ni and 55Fe in Nuclear Waste Samples Using Radiochemical Separation and Liquid Scintillation Counting. Analytical Chimica Acta. 2005;535:297–307.

 

  1. Choi K.C, Park S.K, Han S.H, Choi K.S, Jee K.Y. Determination of 129I in Radioactive Waste from Korea Npps. Proceedings of 10th International Conference on Environmental Remediation and Radioactive Waste Management. 2005:1446–1449.

 

  1. Osvath S, Vajda N, Molnar Z, Kovaca-Szeles E, Braun M, Halasz M. Determination of 93Zr in Nuclear Power Plant Wastes. Journal of Radioanalytical and Nuclear Chemistry. 2017;314:31–38.

 

  1. Guerin N, Gagne A, Kramer-Tremblay S. A rapid method for the routine monitoring of Tc-99 by liquid scintillation counting. Journal of Radioanalytical and Nuclear Chemistry. 2017;314:2009–2017.

 

  1. Vesely A, Trombitas H, Lindauer H. Determination of beta emitters in materials from research reactor decomissioning. In: Eikenberg J, Ja¨ggi M, Beer H, Baehrle H (eds) Advances in liquid scintillation spectrometry. University of Arizona, Radiocarbon Publishers, Tucson. 2008;435–441.

 

  1. Haas P.A. A Review of Information on Ferrocyanide Solids for Removal of Cesium from Solutions. Separation Science and Technology. 1993;28:2479-2506.

 

  1. Remenec B, Dulanska S, Paucova V, Matel L. Determination of 99Tc in Evaporator Concentrates Using Solid Phase Extraction Techniques. Journal of Radioanalytical and Nuclear Chemistry. 2011;290:403–407.

 

  1. Gaca P, Reading D, Warwick P. Application of Multiple Quench Parameters for Confirmation of Radionuclide Identity in Radioanalytical Quality Control. Journal of Radioanalytical and Nuclear Chemistry. 2019;322:1383–1390.

Keywords

Technetium-99
Technetium-99m
Bushehr nuclear power plant waste
Processes yield
Purification
Specific activation
  1. Hou X. Liquid Scintillation Counting for Determination of Radionuclides in Environmental and Nuclear Application. Journal of Radioanalytical and Nuclear Chemistry. 2018;318:1597–1628.

 

  1. Shi K.L, Hou X.L, Roos P, Wu W.S. Determination of Technetium-99 in Environmental Samples: A Review. Analtical Chimica Acta. Analtical Chim Acta. 2011;709:1–20.

 

  1. Rozas S, López J, Idoeta R, Herranz M. Selectivity Analysis of 99Tc Determination by LSC in the Field of Nuclear Decommissioning. Journal of Radioanalytical and Nuclear Chemistry. 2022;331:3335–3341.

 

  1. Butterworth J.C, Livens F.R, Makinson P.R. Development of a Method for the Determination of Low Levels of Technetium-99. The Science of the Total Environment. 1995;173/174:293-300.

 

  1. Reis A.S, Temba E.S.C, Kastner G.F, Monteiro R.P.G. Isolation and Activity Determination of 99Tc in Nuclear Waste by Liquid Scintillation Counting. 2011 International Nuclear Atlantic Conference- INAC. 2011.

 

  1. Chao J.H, Tseng C.L, Lee C.J. Sequential Extraction Separation for Determination of Technetium-99 in Radwastes by ICP-MS. Journal of Radioanalytical and Nuclear Chemistry. 2002:251(1);105-112.

 

  1. Shia K, Houa X, Roosa P, Wub W. Determination of Technetium-99 in Environmental Samples: A review. Analytica Chimica Acta. 2012:709;1–20.

 

  1. Momoshima N, Sayad M, Takashima Y. Analytical Procedure for Technetium-99 in Seawater by ICP-MS. Radiochimca Acta. 1993;63:73–78.

 

  1. Ikaheimonen T.K, Vartti V.P, Ilus E, Mattila J. Technetium-99 in Fucus and Seawater Samples in the Finnish Coastal Area of the Baltic Sea. Journal of Radioanalytical and Nuclear Chemistry. 1999:252:309–313.

 

  1. Goken G.L, Bruening R.L, Krakowiak K.E, Izatt R.M. Metalion Separations Using Superlig or Analig Materials Encased in Empore Cartriges and Disks. ACS Symposium Series 716, American Chemical Society, Washington, DC. 1999;251–529.

 

  1. Izatt S.R, Bruening R.L, Krakowiak K.E, Izatt R.M. The Selective Separation of Anions and Cations in Nuclear Waste Using Commercially Available Molecular Recognition Technology Products. Proceedings of WM’03 Conference, Tuscon. 2003.

 

  1. Remenec B, Dulanska S, Paucova V, Matel L. Determination of 99Tc in Evaporator Concentrates Using Solid Phase Extraction Techniques. Journal of Radioanalytical and Nuclear Chemistry. 2011;290:403–407.

 

  1. Uchida S, Tagami K. Separation and Concentration of Technetium Using A Tc-Selective Extraction Chromatographic Resin. Journal of Radioanalytical and Nuclear Chemistry. 1997;221:35–39.

 

  1. Dixon P, Curtis D.B, Musgrave J, Roensch F, Roach J, Rokop D. Analysis of Naturally Produced Technetium and Plutonium in Geologic Materials. Analalytical Chemistry. 1997;69:1692–1699.

 

  1. Prout W.E. Russell E.R, Groh H.J. Ion Exchange Absorption of Cesium by Potassium Hexacyanocobalt (II) Ferrate (II). Journal of Inorganic and Nuclear Chemistry. 1965;27:473-479.

 

  1. Ru Y, Zheng S, Xue H, Pang H. Potassium Cobalt Hexacyanoferrate Nanocubic Assemblies for High-Performance Aqueous Aluminum Ion Batteries. Chemical Engineering Journal. 2020;382:122853.

 

  1. Hou X.L. Radiochemical Determination of 41Ca in Reactor Concrete for Decommissioning. Radiochimca Acta. 2005;93:611–617.

 

  1. Hou X.L. Radiochemical Analysis of Radionuclides Difficult to Measure or Waste Characterization in Decommissioning of Nuclear Facilities. Journal of Radioanalytical and Nuclear Chemistry. 2007;273:43–48.

 

  1. Hou X.L, Frøsig L, Nielsen S.P. Determination of 36Cl in Nuclear Waste from Reactor Decommissioning. Analalytical Chemistry. 2007;79:3126–3134.

 

  1. Hou X.L, Ostergaard L.F, Nielsen S.P. Determination of 63Ni and 55Fe in Nuclear Waste Samples Using Radiochemical Separation and Liquid Scintillation Counting. Analytical Chimica Acta. 2005;535:297–307.

 

  1. Choi K.C, Park S.K, Han S.H, Choi K.S, Jee K.Y. Determination of 129I in Radioactive Waste from Korea Npps. Proceedings of 10th International Conference on Environmental Remediation and Radioactive Waste Management. 2005:1446–1449.

 

  1. Osvath S, Vajda N, Molnar Z, Kovaca-Szeles E, Braun M, Halasz M. Determination of 93Zr in Nuclear Power Plant Wastes. Journal of Radioanalytical and Nuclear Chemistry. 2017;314:31–38.

 

  1. Guerin N, Gagne A, Kramer-Tremblay S. A rapid method for the routine monitoring of Tc-99 by liquid scintillation counting. Journal of Radioanalytical and Nuclear Chemistry. 2017;314:2009–2017.

 

  1. Vesely A, Trombitas H, Lindauer H. Determination of beta emitters in materials from research reactor decomissioning. In: Eikenberg J, Ja¨ggi M, Beer H, Baehrle H (eds) Advances in liquid scintillation spectrometry. University of Arizona, Radiocarbon Publishers, Tucson. 2008;435–441.

 

  1. Haas P.A. A Review of Information on Ferrocyanide Solids for Removal of Cesium from Solutions. Separation Science and Technology. 1993;28:2479-2506.

 

  1. Remenec B, Dulanska S, Paucova V, Matel L. Determination of 99Tc in Evaporator Concentrates Using Solid Phase Extraction Techniques. Journal of Radioanalytical and Nuclear Chemistry. 2011;290:403–407.

 

  1. Gaca P, Reading D, Warwick P. Application of Multiple Quench Parameters for Confirmation of Radionuclide Identity in Radioanalytical Quality Control. Journal of Radioanalytical and Nuclear Chemistry. 2019;322:1383–1390.

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