A method utilizing extractive scintillating resin for 99Tcmonitoring in aqueous solutions is presented. These extractive scintillatorscombine analyte selective uptake and scintillating properties to produce dualfunctionality analytical resins. These resins were produced by (1) co-locatedextraction chromatographic resin and plastic scintillating beads, (2) immobilizingfluors in macroporous polystyrene supports to which chains of monomethylatedpolyethylene glycol have been grafted and (3) co-immobilizing organic scintillatingfluors and a quaternary ammonium extractant (Aliquat-336) within macroporousacrylic and polystyrene supports. The first and third resins selectively extractpertechnetate ions from dilute acid whereas the second resin selectively extractspertechnetate ions from high ionic strength solutions. These resins were utilizedin ~0.20 ml pore volume columns while 99Tc was continually monitoredwith commercially available scintillation detection systems. Manual and automatedmicrofluidics were used to deliver sample and reagent solution for loadingand elution of the 99Tc. The detection efficiencies were determinedto be 45 and 70% for acrylic and polystyrene based resins, respectively, andindependent of extractant. Minimum detectable 99Tc concentrationusing the Aliquat-336/acrylic-based resin was 6.2 Bq . l –1 for a 50-mlsample and 30-minute count time. The new methodology was applied towards analysisof contaminated groundwater samples and nuclear waste simulants.
Authors:O. B. Egorov, M. J. O’Hara, and J. W. Grate
A fully automated analysis procedure and instrument for the measurement of total 99Tc in aged nuclear waste has been developed. The overall analysis approach is based on a fully automated wet radiochemical analysis method. Microwave-assisted sample oxidation is used prior to a chemical separation step in order to oxidize all of the non-pertechnetate species to pertechnetate. Separation of the pertechnetate from interfering radioactive and stable matrix species is carried out using an anion-exchange column. The separated 99Tc is quantified using a flow-through solid cell scintillation detector. The instrument is capable of an analysis time of <13 minute per sample with a detection limit of 2000 dpm/ml. Nuclear waste samples from the Hanford site with a high content of non-pertechnetate species were successfully analyzed using this method.
Authors:R. S. Addleman, M. J. O’Hara, J. W. Grate, and O. B. Egorov
Direct alpha-energy spectroscopy in liquids is possible by placing a chemically selective polymer thin film upon the surface of passivated silicon diodes. By utilizing polymer thin films with high affinity for actinides, we have been able to selectively concentrate actinides of interest upon the diode surface, resulting in a substantial increase in sensitivity relative to a direct measurement. With this film coated diodes, we were able to obtain in-situ alpha spectra with energy resolution comparable to that of conventional alpha-spectroscopy. The response of the thin film coated diode was found to be linear over 104. The sensitivity and reversibility is a function of the membrane complexation chemistry.
Authors:R. S. Addleman, M. J. O’Hara, T. Marks, J. W. Grate, and O. B. Egorov
The determination of transuranic (TRU) content in nuclear wastes, reactor materials, process solutions, and various other matrices is required in support of material assessment, environmental restoration, and waste processing activities. We have found that direct measurement of TRU is possible using surface passivated ion implanted planar silicon diode detectors. The performance and durability of modern silicon diodes enables direct detection of alpha-particles, with retention of some spectral information, through small air gaps or under direct contact with liquid or solid samples. We will present results on the performance of silicon diode detectors for the determination of TRU in liquids.