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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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