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A European Perspective on the Use of Eichrom Resins

A European Perspective on the Use of Eichrom Resins. Dr Jon Martin BNFL. BNFL UK Sites. Hunterston A. Chapelcross. Calder Hall. Sellafield. Risley HQ. Wylfa. Maentwrog. Trawsfynydd. Sizewell A. Berkeley. Bradwell. Hinkley Point A. Oldbury. Littlebrook. Dungeness A.

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A European Perspective on the Use of Eichrom Resins

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  1. A European Perspective on theUse of Eichrom Resins Dr Jon Martin BNFL

  2. BNFL UK Sites Hunterston A Chapelcross Calder Hall Sellafield Risley HQ Wylfa Maentwrog Trawsfynydd Sizewell A Berkeley Bradwell Hinkley Point A Oldbury Littlebrook Dungeness A

  3. An Overview (1992-1998) • Background • Initial use in emergency response planning. • Application to simple matrices. • A difficult problem - resolved with Ln.Resin. • Application to environmental matrices. • Accreditation for plant-support methods. • The broader picture.

  4. CRL Lab Overview Central Radiochemical Laboratory Environment Liquid & Gaseous Effluent Magnox AGR Low Level Waste Waste Characterisation Lab. Decommissioning Lab. Intermediate Level Waste

  5. Extraction Chromatography - Application to Emergency Methods “The aftermath of an accident is not a time to begin the development of novel procedures”. N. Green, NRPB • EEC Intervention Levels: Material Limiting Activity Concentration Sr-89/Sr-90 Pu-239, Am- Others with t >10 1/2 241, Cm-242/4 days (excl. H-3 / C-14 Dairy produce & 125 20 1000 liquid foods ( Bq/kg) Solid & Liquid 750 80 1250 Foods ( Bq/kg)

  6. Sequential Emergency Procedure Add radionuclide spikes Microwave digest Anion exchange column Electrodeposit or Sr , Am, Cm not coppt Pu retained Am, Cm fraction to Sr .Resin TRU.Resin Sr -89/90 Coppt Am / Cm determination source

  7. Rapid Sr-89 / 90 Procedure Elute from Sr .Resin in 8ml water Cerenkov count (15min) Sr -85 yield determination Add Ultima Gold XR Liquid scint . count Calculation of Sr -89 & Sr -90 - Correction for Y-90

  8. Limitations Merits • Sample size. • Large excess of Am-241 over Am-243 yield tracer. • Uranium breakthrough in Pu spectrum. • Batch size dominated by microwave digestion. • Sampling uncertainty. • <24 hour turnaround, incl. Screening of 80 samples & analysis of 6. • Addresses required limits of detection and accuracy. • Introduced the benefits of extraction chromatography…

  9. Summary of routinemethodology…1 Analysis Classical separation Extraction Comments chromatography Tritium Distillation Tritium.Resin investigated but clean-up not sufficient for Magnox effluent. C-14 Wet / dry oxidation S-35 Wet oxidation and chemical isolation and / or cation exchange C1-36 Chemical isolation Ca-45 Chemical isolation Sr.Resin + classical RE.Resin investigated chemistry but little Mn-54 clean-up Mn-54 Chemical isolation Fe-55 Solvent extraction Ni-63 Ni.Resin

  10. Analysis Classical Extraction separation chromatography Summary of routinemethodology…2 Comments Sr.Resin Excepting large volume milk Sr-90 / Sr- samples 89 Tc-99 TEVA.Resin Low requirement Solvent extraction ABEC.Resin Extraction chromatography not I-129 normally necessary Pm-147 Ln.Resin Sm-151 Pb-210 Sr.Resin Distillation or direct Sr.Resin Po-210 auto deposition Ra-226 U/ TEVA.Resin / Uranium / TEVA Resin Thorium Transuranics TEVA / TRU. Resins

  11. Pm-147 / Sm-151Analysis...Why? Pm-147 • High abundance in fresh fission product mixtures. Sm-151 • Increasing importance in decayed fission product mixtures. • Pure soft -active radionuclides. • Radiotoxicity comparable to that of carbon-14. What yield tracer? • No suitable isotopic yield tracer. • No naturally occuring isotope. • No suitable isotopic yield tracer. • Gravimetric yield determination possible.

  12. Assessment of ‘Low Abundance’ Isotopes' compliance with de minimis Criteria for Disposal Radionuclide Maximum Theorectical de minimis Activity per Consignment Se-79 0.0075 13 Y-91 10300 13 Zr-93 0.0047 13 Nb-93m 0.029 13 Tc-99 0.37 13 Pd-107 0.002 13 Sn-126 0.28 13 I-129 0.00069 0.05 Cs-135 0.019 13 Sm-151 6.3 13

  13. Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Pm-147 / Sm-151 Analysis...Interferences b Ho-166m [1200y, ] b/g, Eu -154 [8.59y, 580 keV ] ........1.9 b/g, Eu -155 [4.85y, 160 keV ] ........2.6 . to Cs-137 (%) b, Sm -151 [88.7y, 76 keV ] .....................0.31 b, @ 5GWd/T, 4 years decayed Pm -147 [2.6y, 225 keV ] .............................79 rel g, Pr-144 [285d, 2.996 keV ] Abundance b, Ce -144 [285d, 318 keV ] ..........................................................23

  14. Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Pm-147 Analysis...Yield tracers a Natural Samarium Gd -148, [3.27 MeV ] a ...natural Natural Neodymium a ...natural

  15. Promethium-147 by Eichrom’s Ln.Resin • Ln.Resin - not to be confused with RE.Resin (of course!) • HDEPH: bis(2-ethylhexyl) phosphoric acid supported on Amberchrom CG-71 at a 40%w/w loading. • Original work by Horwitz & Bloomquist, J. Inorg. Nucl. Chem. 17, 425 (1975).

  16. Pm-147 / Sm-151Analysis...Gd-148 yield tracer 1.0 0.9 0.15 M nitric acid 0.25 M nitric acid 0.4 M nitric acid 0.8 Eu 0.7 Am Am Gd 0.6 Normalised count rate (Arb) 0.5 Pm 0.4 0.3 0.2 0.1 0.0 0 10 20 30 40 50 60 70 3 Volume (cm )

  17. Pm-147 / Sm-151 Analysis...Natural Sm yield tracer 1.0 0.9 0.8 0.7 0.6 Normalised count rate / Sm concentration (Arb) 0.5 0.4 0.3 0.2 0.1 0.0 0 50 100 150 200 250 300 3 Volume (cm )

  18. Summary of Pm-147 / Sm – 151 Results Sample Pm-147 Result Sm-151 Result Ratio description FMDT liquid effluent 698 + 49 9.28 + 2.83 75 + 24 annual bulk (15/06/97) mean of 4 results AETP sludge 2.40 + 0.20 1.92 + 0.22 1.25 + 0.18 dissolution liquor – A AETP sludge 1.35 + 0.15 0.949 + 0.099 1.42 + 0.22 dissolution liquor – B ILW resin sample 18.3 + 1.4 13.0 + 1.0 1.41 + 0.15 (Lewatit DN) LLW QC spiked (-2.8 + 10.8)% solution

  19. Benefits • Approximate 60% cost reduction per analysis through time savings and larger batches. • Fully validated, accredited methods with comprehensive uncertainty budgets. • Methods proven at national and international intercomparison exercises.

  20. Environmental / Bioassay Matrices - Overcoming the Interferences • Sr-90 in fish, urine, faecal ash. • 3g Sr.Resin in column. • Pu / Am in soils. • Anion exchange pre-clean-up. • Preliminary work on pre-concentration of transuranics on Diphonix, followed by Fenton’s Reagent destruction of organics - see work by Bill Burnett, FSU.

  21. Application of Eichrom technology to other BNFL processes • Support to reprocessing: product quality and accountancy. • Tc-99 analysis - TEVA - various matrices. • Environmental monitoring programmes. Application of Eichrom technology in Europe Mature processes which are broadly used in a wide range of applications. PROCORAD - laboratories from >20 countries. Many used Eichrom extractants.

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