Nick Soelberg

Radioactive Iodine and Krypton Control for Nuclear Fuel Reprocessing Facilities

The removal of volatile radionuclides generated during used nuclear fuel reprocessing in the US is almost certain to be necessary for the licensing of a reprocessing facility in the US. Various control technologies have been developed, tested, or used over the past 50 years for control of volatile radionuclide emissions from used fuel reprocessing plants. The US DOE has sponsored, since 2009, an Off-gas Sigma Team to perform research and development focused on the most pressing volatile radionuclide control and immobilization problems. In this paper, we focus on the control requirements and methodologies for 85Kr and 129I. Numerous candidate technologies have been studied and developed at laboratory and pilot-plant scales in an effort to meet the need for high iodine control efficiency and to advance alternatives to cryogenic separations for krypton control. Several of these show promising results. Iodine decontamination factors as high as 105, iodine loading capacities, and other adsorption parameters including adsorption rates have been demonstrated under some conditions for both silver zeolite (AgZ) and Ag-functionalized aerogel. Sorbents, including an engineered form of AgZ and selected metal organic framework materials (MOFs), have been successfully demonstrated to capture Kr and Xe without the need for separations at cryogenic temperatures.

Deep Bed Adsorption Testing using Silver-Functionalized Aerogel

Nuclear fission results in the production of fission products and activation products, some of which tend to be volatile during used fuel reprocessing and evolve in gaseous species into the reprocessing facility off-gas systems. Analyses have shown that I129, due to its radioactivity, high potential mobility in the environment, and high longevity (half life of 15.7 million years), can require control efficiencies of up to 1,000x or higher to meet regulatory emission limits. Two Aerogel sorption tests that have been performed this fiscal year. The maximum iodine decontamination factor (DF) was measured to be over 10,000, above the 1,000-10,000 target DF range. The mass transfer zone may be as short as 0.5 inches under the sorption conditions of the first test. Only a small fraction of the iodine sorbed on Bed 1 was desorbed during the purge periods. The silver-functionalized Aerogel appears to have potential to be a very effective and efficient iodine sorbent.

Performance Criteria for Capture and/or Immobilization Technologies - Milestone Report

The capture and subsequent immobilization of the four regulated volatile radionuclides (3H, 14C, 85Kr, and 129I) from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international colleagues. Removal of some or all of these radionuclides (e.g., based upon fuel burnup, fuel type, cooling time) from the plant effluent streams prior to discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclide, as well as associated sorbents that cannot be cost-effectively regenerated, is destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technologies, including liquid caustic scrubbing systems, solid adsorbents, and cryogenic distillation. The studies of waste forms have been correspondingly diverse. In considering the technologies available for future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to evaluate objectively each sorbent system or waste form.

Studies on the Mechanisms of Methyl Iodide Adsorption and Iodine Retention on Silver-Mordenite

Silver-containing mordenite (MOR) is a longstanding benchmark for radioiodine capture, reacting with molecular iodine (I2) to form AgI. However the mechanisms for organoiodine capture are not well understood. Here we investigate the capture of methyl iodide from complex mixed gas streams by combining chemical analysis of the effluent gas stream with in depth characterization of the recovered sorbent.

CARBON BED MERCURY EMISSIONS CONTROL FOR MIXED WASTE TREATMENT

Abstract Mercury has various uses in nuclear fuel reprocessing and other nuclear processes, and so it is often present in radioactive and mixed (radioactive and hazardous) wastes. Compliance with air emission regulations such as the Hazardous Waste Combustor (HWC) Maximum Achievable Control Technology (MACT) standards can require off-gas mercury removal efficiencies up to 99.999% for thermally treating some mixed waste streams. Test programs have demonstrated this level of off-gas mercury control using fixed beds of granular sulfur-impregnated activated carbon. Other results of these tests include (1) the depth of the mercury control mass transfer zone was less than 15–30 cm for the operating conditions of these tests; (2) MERSORB® carbon can sorb mercury up to 19 wt % of the carbon mass; and (3) the spent carbon retained almost all (98.3–99.99%) of the mercury during Toxicity Characteristic Leachability Procedure (TCLP) tests, but when even a small fraction of the total mercury dissolves, the spent carbon can fail the TCLP test when the spent carbon contains high mercury concentrations.