1 / 26

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

betty_james
Télécharger la présentation

Chromatographic Separation and Measurement of Charged-Particle Emitting Radionuclides

An Image/Link below is provided (as is) to download presentation Download Policy: Content on the Website is provided to you AS IS for your information and personal use and may not be sold / licensed / shared on other websites without getting consent from its author. Content is provided to you AS IS for your information and personal use only. Download presentation by click this link. While downloading, if for some reason you are not able to download a presentation, the publisher may have deleted the file from their server. During download, if you can't get a presentation, the file might be deleted by the publisher.

E N D

Presentation Transcript

  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

More Related