The efficient capture of radioactive methyl iodide (CH3131I) is a critical issue for nuclear safety and radioprotection. Co-impregnated activated carbons (AC), with triethylenediamine (TEDA) and potassium iodide (K127I), are widely employed for this purpose. However, the specific role of KI in CH3131I retention through isotopic exchange reaction remains poorly understood. This study provides groundbreaking insights by systematically investigating the retention behavior of KI/AC versus non-impregnated activated carbons (NI AC) under different operating conditions. Advanced characterization techniques, including N2 porosimetry, high-resolution transmission electron microscopy (HRTEM), and H2O adsorption isotherms, were first employed to elucidate the structural and chemical properties of the adsorbents. Subsequently, CH3131I retention tests were conducted by measuring the Decontamination Factors (DF) at various configurations covering a broad range of relative humidities (RH) (20–90 %), temperatures (20–96 °C), residence times (0.125–0.5 s) and elution times (1–18 h). Results reveal that while NI AC exhibits a drastic performance decline at high RH attributable to water physisorption, KI/AC demonstrates enhanced retention, counterbalancing moisture effects via isotopic exchange. Furthermore, elevated temperatures significantly amplify DF for KI/AC, unveiling for the first time the thermally activated nature of the isotopic exchange mechanism. Prolonged residence time further enhance performance for KI/AC compared to NI AC, suggesting multiple mechanistic steps in isotopic exchange reaction. Consequently, a detailed mechanism for this reaction has been proposed.
This work advances the understanding of CH3131I capture mechanisms ensuring improved performance under diverse nuclear safety scenarios.