Automated Radioanalytical System Incorporating Microwave- Assisted Sample Preparation, Chemical Separation, and Online Radiometric Detection for the Monitoring of Total ~(99)Tc in Nuclear Waste Processing Streams

摘要

An automated fluidic instrument is described that rapidly determines the total ~(99)Tc content of aged nuclear waste samples, where the matrix is chemically and radiologically complex and the existing speciation of the ~(99)Tc is variable. The monitor links microwave-assisted sample preparation with an automated anion exchange column separation and detection using a flow-through solid scintillator detector. The sample preparation steps acidify the sample, decompose organics, and convert all Tc species to the pertechnetate anion. The column-based anion exchange procedure separates the pertechnetate from the complex sample matrix, so that radiometric detection can provide accurate measurement of ~(99)Tc. We developed a preprogrammed spike addition procedure to automatically determine matrix-matched calibration. The overall measurement efficiency that is determined simultaneously provides a self-diagnostic parameter for the radiochemical separation and overall instrument function. Continuous, automated operation was demonstrated over the course of 54 h, which resulted in the analysis of 215 samples plus 54 hly spike-addition samples, with consistent overall measurement efficiency for the operation of the monitor. A sample can be processed and measured automatically in just 12.5 min with a detection limit of 23.5 Bq/mL of ~(99)Tc in low activity waste (0.495 mL sample volume), with better than 10 percent RSD precision at concentrations above the quantification limit. This rapid automated analysis method was developed to support nuclear waste processing operations planned for the Hanford nuclear site.