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Chromatographic Separation and Measurement of Charged-Particle Emitting Radionuclides

Chromatographic Separation and Measurement of Charged-Particle Emitting Radionuclides. Timothy A. DeVol, Ph.D., C.H.P. Environmental Engineering and Science Clemson University 16 May 2000. Introduction to Dual Functionality Materials. Liquid Extractive Scintillators

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Chromatographic Separation and Measurement of Charged-Particle Emitting Radionuclides

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  1. Chromatographic Separation and Measurement of Charged-Particle Emitting Radionuclides Timothy A. DeVol, Ph.D., C.H.P. Environmental Engineering and Science Clemson University 16 May 2000

  2. Introduction to Dual Functionality Materials • Liquid Extractive Scintillators • Ludwick, Health Physics, 1961, 6, 63-65. • McDowell and McDowell, Liquid Scintillation Alpha Spectrometry, CRC Press, Boca Raton, 1994. • Scintillating Cation and Anion Ion Exchange Resin • Heimbuch, et al., Radioisotope Sample Measurement Techniques in Medicine and Biology, Proceedings of the International Atomic Energy Agency Symposium, Vienna, May 24-28, 1965. • Solid Extractive Scintillators for 90Sr and 99Tc • Egorov et al., Anal. Chem 71 (1999) 5420-5429 • Solid Extractive Scintillators for 90Sr, 99TcandActinides • DeVol et al., Radioactivity&Radiochemistry Vol. 11 #1 (2000)

  3. Separation and Detection Schemes • Single scintillation crystal, e.g. CaF2:Eu, anthracene • Extractant coated onto inert scintillator • Mixture of extraction resin with granular scintillator • Extractant impregnated into a scintillating chromatographic resin (ScintEx)

  4. Solid Extractive Scintillators • Sequential Extraction Chromatography and Flow-cell Detection Off-line quantification • Simultaneous Extraction Chromatography and Flow-cell Detection On-line quantification

  5. Materials and Methods • Mixed-ResinMixture of: • 100 - 150 mm TEVA Resin or Sr Resin • 100 - 200 mm BC-400 Plastic Scintillation Beads (Bicron)or 63 - 90 mm GS-20 Scintillating Glass (Applied Scintillation Technology)

  6. Extractive Scintillator Resin • ScintEx resin (Patent Pending) • Inert polystyrene chromatographic resin (Amberchrom CG-161c) impregnated with PPO and DM-POPOP using a modification of the Ross 1991 procedure • Scintillating chromatographic bead impregnated with extractant (Eichrom proprietary technology) • Extractant for Sr • ABEC-2000 • Quaternary Amine, Aliquat-336 (TEVA) • CMPO extractant in TBP for actinides

  7. Off-Line Evaluation Procedures • Resin dry packed into 9 mm x 50 mm opaque column • Conditioning, loading and wash performed with standard Eichrom procedures • Column placed in 7-mL HDPE vial WITHOUT introduction of LSC cocktail • Activity quantified with Hidex Triathler liquid scintillator counter

  8. Hidex Triathler

  9. Results and Discussion • Mini-Column Experiments (Off-Line) • Compare pulse-height spectra (luminosity) and detection efficiency • Flow-Cell Experiments (On-Line) • Loading and elution profiles (loading and detection efficiency, and total recovery) • Regeneration capability

  10. 89Sr Pulse-Height Spectra from Triathler

  11. Triathler Pulse-Height Spectra for 89Sr and 90Sr on Sr ScintEx O

  12. PMT PMT Schematic of On-Line Flow-Cell Detection System Flow-cell Manually controlled pump Radiation Detector Effluent Loading Solution Eluant Sample Computer LSC

  13. Flow-Cell Radiation Detection System IN/US b-Ram Model 1

  14. Extractive Scintillator Flow-Cell Extractive scintillator flow-cell was constructed of with <0.5 g of resin packed into 1.5 mm ID x 140 mm polytetrafluoro- ethylene tubing to yield an approximate pore volume of 200-400 mL. The tubing is coiled to an approximate diameter of 2.54 cm and placed between the photomultiplier tubes of the radiation detector.

  15. Loading and Elution of 99Tc(VII)TEVA/BC-400 Mixed Resin e(99Tc) = 7.5%

  16. Loading and Elution of 99TcTEVA/BC-400 Mixed-Resin Flow-Cell137Cs Interference Test 99Tc; 5 mL; 24 Bq mL-1 137Cs; 1 mL; 7.2 kBq mL-1

  17. Loading and Elution of 99TcABEC ScintEx Flow-Cell

  18. Loading and Elution of 99TcTEVA ScintEx Flow-Cell

  19. Loading and Regeneration of TEVA ScintEx

  20. 89Sr Loading and Elution Profile on Sr ScintEx O e (89Sr) = 65.4%

  21. Loading 90Sr/90Y on Sr ScintEx P 102 e (90Sr)= 40%

  22. Multiple Loading and Elution of 89Sr on Sr ScintEx O Avg. Detection efficiency 60  4% Avg. Loading efficiency 101 ± 1% 65.4% 58.8% 57.6% 59.6%

  23. TRU ScintEx ResinPulse Height Spectrum

  24. Sequential Elution of 241Am, 239Pu and 233U from TRU ScintEx Resin On-Line Counting Off-Line Counting

  25. Conclusions • Extractive scintillator media can be realized a number of ways • Extractive scintillator media can be selective to analyte of interest • demonstrated with technetium-selective, strontium-selective and actinide-selective extractant • Loading, retention, and elution similar to non-scintillating resin • Quantification has been demonstrated on-line and off-line • Limited spectroscopy appears to be available with the actinide-selective ScintEx resin • Absolute detection efficiency ranges from ~40% for 90Sr to near 100% for actinide- selective ScintEx resin

  26. Acknowledgments • James Harvey, Eichrom IndustriesJonathan Duffey, formerly from Eichrom • From Clemson University:Robert Fjeld, Alena Paulenova (on leave from Comenius´ University, Slovak Republic), James Roane • John Leyba, WSRTC • NSF SBIR Phase I contract # NSF/SBIR-9760934 • South Carolina University Education and Research Foundation TOA #KC86372-O. • DOE Environmental Management and Science Program, Project #70179

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