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Selective metal extraction from solid matrices with TBP complex with nitric acid in supercritical carbon oxide

Research Project

Project/Area Number 13480145
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Nuclear engineering
Research InstitutionNagoya University

Principal Investigator

ENOKIDA Youichi  Nagoya University, Research Center for Nuclear Materials Recycle, Professor, 環境量子リサイクル研究センター, 教授 (40168795)

Co-Investigator(Kenkyū-buntansha) TSUSHIMA Satoru  Nagoya University, Department of Nuclear Engineering, Associate Professor, 工学研究科, 助教授 (80312990)
YAMAMOTO Ichiro  Nagoya University, Department of Nuclear Engineering, Professor, 工学研究科, 教授 (50023320)
Project Period (FY) 2001 – 2003
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥12,400,000 (Direct Cost: ¥12,400,000)
Fiscal Year 2003: ¥1,900,000 (Direct Cost: ¥1,900,000)
Fiscal Year 2002: ¥5,000,000 (Direct Cost: ¥5,000,000)
Fiscal Year 2001: ¥5,500,000 (Direct Cost: ¥5,500,000)
Keywordslanthanides / metal extraction / tri-n-butylphosphate / supercritical fluid / nitric acid complex / carbon dioxide / ultrasound / 超音波 / 超臨界流体抽出 / 環境調和
Research Abstract

Selective recovery of lanthanide elements from a mixture of metal oxides was demonstrated using tri-n-butylphosphate complex with nitric acid and water dissolved in supercritical carbon dioxide (SF-CO_2). Recovery yields were experimentally evaluated under various temperatures and pressures ; influences of temperature and pressure were studied and optimum conditions for metal extraction were determined. Higher temperature is preferable for rapid dissolution because of activation energy. Concerning with pressure, the optimum value exists because density becomes larger, but mole fraction of the complex decreases as pressure increases. The optimal pressure is very close to the critical point for the mixture of the complex, and SF-CO_2. To study mechanisms of selective dissolution and extraction of metals form their oxides, dissolution and extraction rates was correlated with the mole ratios of TBP/HNO_3/H_2O and a fact that, the higher ratios of HNO_3/TBP and, H_2O/TBP are preferable was found. ^3H-NMR measurements on TBP complex supports that TBP complex contains a solvent structure of reverse micelle like. It was also found that ultrasound application is so effective that it may enhance the extraction rates ten times larger than without its application. The solubility of TBP complex in SF-CO_2 was well predicted by a molecular simulation.

Report

(4 results)
  • 2003 Annual Research Report   Final Research Report Summary
  • 2002 Annual Research Report
  • 2001 Annual Research Report
  • Research Products

    (30 results)

All Other

All Publications (30 results)

  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "New method for the removal of uranium from solid wastes with supercritical CO2 medium containing HNO_3-TBP complex"Journal of Nuclear Science and Technology. 38. 461-462 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "Dissolution behavior of uranium oxides with supercritical CO2 using HNO3-TBP complex as a reactant"Journal of Nuclear Science and Technology. 39. 1097-1102 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto: "Selective recovery of neodymium from oxides by direct extraction method with supercritical CO_2 containing TBP-HNO_3 complex"Separation Science and Technology. 37. 1153-1162 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida et al.: "Ultrasound Enhanced Dissolution of UO2 in Supercritical CO2 Containing a CO2-Philic Complexant of Tri-n-butylphosphate and Nitric Acid"Industrial and Engineering Chemistry Research. 41. 2282-2286 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida, I.Yamamoto: "Vapor-liquid equilibrium of UO_2(NO_3)_22TBP and supercritical carbon dioxide mixture"Journal of Nuclear Science and Technology. Supp.3. 270-273 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida et al.(分担執筆): "Separations and Processes using Supercritical Carbon Dioxide"American Chemical Society. 479 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "New method for the removal of uranium from solid wastes with supercritical CO_2 medium containing HNO_3-TBP complex"Journal of Nuclear Science and Technology. 38. 461-462 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "Dissolution behavior of uranium oxides with supercritical CO_2 using HNO_3-TBP complex as a reactant"Journal of Nuclear Science and Technology. 39. 1097-1102 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto: "Selective recovery of neodymium from oxides by direct extraction method with supercritical CO_2 containing TBP-HNO_3 complex"Separation Science and Technology. 37. 1153-1162 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida et al.: "Ultrasound enhanced dissolution of UO_2 in supercritical CO_2 containing a CO_2phillic complexant of tri-n-butylphosphate and nitric acid"Industrial and Engineering Chemistry Research. 41. 2282-2286 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida et al.: "Separation and processes using supercritical carbon dioxide"American Chemical Society, ACS Symposium Series. 479 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Y.Enokida et al.: "Characterization of a tri-n-butyl phosphate-nitric acid complex : a CO_2-soluble extractant for dissolution of uranium dioxide"Industrial and Engineering Chemistry Research. 42. 5037-5041 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] R.Shimizu, K.Sawada, Y.Enokida, I.Yamamoto: "Supercritical fluid extraction of rare earth elements from luminescent material in waste fluorescent lamp"Proceedings of the Second International Symposium on Supercritical Fluid Technology for Energy and Environment Application. 1. 323-327 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Sawada, O.Tomioka, Y.Enokida, I.Yamamoto et al.: "Density of supercritical fluid containing UO_2(NO_3)_2-TBP complex and CO_2"Proceedings of Global 2003. 1. 707-710 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 澤田佳代, 宇留賀和義, 榎田洋一他: "超臨界二酸化炭素中でのTBP硝酸錯体による酸化ウランの溶解反応"日本原子力学会中部支部第35回研究発表会要旨集. 1. 40-40 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 今井 誠, 澤田佳代, 津島 悟, 榎田洋一, 山本一良: "リン酸トリブチルに抽出された硝酸ネオジムの水相への物質移動係数"日本原子力学会中部支部第35回研究発表会要旨集. 1. 42-42 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] (20) 松川清和, 澤田佳代, 津島悟, 榎田洋一, 山本一良: "マイクロリアクター内部における2相間の硝酸及びネオジムの物質移動特性"日本原子力学会中部支部第35回研究発表会要旨集. 1. 38-38 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Enokida et al.(分担執筆): "Separations and Processes using Supercritical Carbon Dioxide"American Chemical Society. 479 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Enokida et al.: "Ultrasound Enhanced Dissolution of UO_2 in Supercritical CO_2 Containing a CO_2-Philic Complexant of Tri-n-butylphosphate and Nitric Acid"Industrial and Engineering Chemistry Research. 41. 2282-2286 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto: "Selective Recovery of Neodymium from Oxides by Direct Extraction Method with Supercritical CO_2 Containing TBP-HNO_3 Complex"Separation Science and Technology. 37. 1153-1162 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Enokida, I.Yamamoto: "Vapor-liquid equilibrium of UO_2(NO_3)_2 2TBP and Supercritical Carbon Dioxide Mixture"Journal of Nuclear Science and Technology. 39・Sup.3. 270-273 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Enokida: "Extraction of Uranium and Lanthanides from Their Oxides with TBP-HNO_3-H_2O-CO_2"Abstracts of Papers of the American Chemical Society. IEC Part1. 218 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Enokida: "Application of Supercritical Fluid Extraction to Nuclear Fuel Reprocessing in Japan"Proceedings of the 1st International Symposium on Supercritical Fluid Technology for Energy and Environment Applications. 1. 35-41 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Enokida et al.(分担執筆): "Uranium Extraction from Nuclear Wastes with a High Pressure Mixture of CO_2 and TBP Complex with Nitric Acid"Proceedings of 9th Biennial International Conference on Nuclear and Hazardous Waste Management. (CD-ROM). 1-6 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Enokida et al.: "Separations and Processes using Supercritical Carbon Dioxide"American Chemical Society (in press). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "New method for the removal of uranium from solid wastes with supercritical CO2 medium containig HNO3-TBP complex"Journal of Nuclear Science and Technology. 38(6). 461-462 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto et al.: "Dissolution behavior of uranium oxides with supercritical CO2 using HNO3-TBP complex as a reactant"Journal of Nuclear Science and Technology. 38(12). 1097-1102 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] O.Tomioka, Y.Enokida, I.Yamamoto: "Selective recovery of neodymium from oxides by direct extraction method with supercritical CO2 containing TBP-HNO3 complex"Separation Science and Technology. (in press). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Enokida et al.: "Ultrasound Enhanced Dissolution of UO2 in Supercritical CO2 Containing a CO2-Philic Complexant of Tri-n-butylphosphate and Nitric Acid"Industrial and Engineering Chemistry Research. (in press). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Enokida, I.Yamamoto: "Vapor-liquid equilibrium of UO2(NO3)2 2TBP and supercritical carbon dioxide mixture"Journal of Nuclear Science and Technology. (in press). (2002)

    • Related Report
      2001 Annual Research Report

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Published: 2001-04-01   Modified: 2016-04-21  

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