Iodine Adsorption by Ag-Aerogel under Prototypical Vessel Off-Gas Conditions

U.S. regulations will require the removal of ¹²⁹I from the off-gas streams of any used nuclear fuel (UNF) reprocessing plant prior to discharge of the off-gas to the environment. The required plant decontamination factor for iodine will vary based on fuel burnup, cooling time, and other factors but is very likely to be >1000 and could be as high as 8000. Multiple off-gas streams within a UNF reprocessing plant combine prior to environmental release, and each of these streams contains some amount of iodine. To achieve the decontamination factors (DFs) that are likely to be required by regulations, iodine removal from the vessel off-gas will be necessary. The vessel off-gas contains iodine at very dilute concentrations (ppb levels), and will also contain water vapor. Iodine species present are likely to include both elemental and organic iodides. There will also be solvent vapors and volatile radiolysis products. The United States has considered the use of silver-based sorbents for removal of iodine from UNF off-gas streams, but little is known about the behavior of those sorbents at very dilute iodine concentrations. The purpose of this study was to expose silver-functionalized silica aerogel (AgAerogel) to a prototypical vessel off-gas stream containing 40 ppb methyl iodide to obtain information about organic iodine capture by silver-sorbents at very low iodine concentrations. The design of this extended duration testing was such that information about the rate of adsorption, the penetration of the iodine species, and the overall system DF could be obtained. Results show that CH₃I penetrates into a AgAerogel sorbent bed to a depth of 3.9 cm under prototypical vessel off-gas conditions. An iodine loading of 22 mg I/g AgAerogel was observed in the first 0.3 cm of the bed. Of the iodine delivered to the system, 48% could not be accounted for, and future efforts will investigate this concern. Direct calculation of the decontamination factor is not possible, as no iodine was observed to break through the sorbent beds. Continued studies on the adsorption of iodine from prototypical vessel off-gas streams by silver-based sorbents will attempt to resolve some of the questions raised here, both regarding mass balance and the effect of aging on iodine adsorption by AgAerogel from a dilute gas stream. Additionally, the adsorption of different iodine species, such as I₂ and C₁₂H₂₅I will be studied. Other variables that merit examination are the gas velocity of the test and the dependence of the observed results on the inlet iodine concentration. Finally, longer duration testing should be considered in an effort to determine the mass transfer zone associated with iodine adsorption by AgAerogel under prototypical vessel off-gas conditions. The estimation of mass transfer zone is required for any future industrial implementation.