Sericitization of illite decreases sorption capabilities for cesium

Release of radioactive cesium (137Cs) to environment occurs through nuclear accidents such as Chernobyl and Fukushima. The concern is that 137Cs has long half-life (t1/2 = 30.2 years) with chemical toxicity and γ-radiation. Sorption techniques are mainly applied to remove 137Cs from aquatic environment. In particular, it has been known well that clay minerals (e.g, illite) are effective and economical sorbents for 137Cs. Illite that was formed by hydrothermal alteration exist with sericite through "sericitization" processes. Although sericite has analogous composition and lattice structure with illite, the sorptive characteristics of illite and sericite for radiocesium could be different. This study evaluated the effects of hydrothermal alteration and weathering process on illite cesium sorption properties. Natural illite samples were collected at Yeongdong area in Korea as the world-largest hydrothermal deposits for illite. The samples were analyzed by XRF, XRD and SEM-EDX to determine mineralogy, chemical compositions and morphological characteristics, and used for batch sorption experiments. The Yeongdong illites predominantly consist of illite, sericite, quartz, and albite. The measured cesium sorption distribution coefficients (Kd,Cs) of reference illite and sericite were approximately 6000 and 400 L kg-1 at low aqueous concentration (Cw 10-7 M), respectively. In contrast, Kd,Cs values for the Yeongdong illite samples ranged from 500 to 4000 L kg-1 at identical concentration. The observed narrow and sharp XRD peak of sericite indicated that the sericite has better crystallinity compared to illite. These experimental results suggested that sericitization processes of illite can decline the sorption capabilities of illite for cesium under various hydrothermal conditions. In particular, weathering experiments raised the cesium sorption to illite, which seems to be related to the increase of preferential sorption sites for cesium through crystallinity destruction (i.e., frayed edge sites).