Through collaborative efforts at Texas A&M University and Sandia National Laboratories, a crystalline silicotitanate (CST), which shows extremely high selectivity for radioactive cesium removal in highly concentrated sodium solutions, was synthesized. The effect of hydrogen peroxide on a CST under cesium ion exchange conditions has been investigated. The experimental results with hydrogen peroxide showed that the distribution coefficient of cesium decreased and the tetragonal phase, the major component of CST, slowly dissolved at hydrogen peroxide concentrations greater than 1 M. A simple and novel experimental apparatus for a single-layer ion exchange column was developed to generate experimental data for estimation of the intraparticle effective diffusivity. A mathematical model is presented for estimation of effective diffusivities for a single-layer column of CST granules. The intraparticle effective diffusivity for Cs was estimated as a parameter in the analytical solution. By using the least square method, the effective diffusivities of 1.56 ± 0.14 x 10-11 m2/s and 0.68 ± 0.09x 10-11 m2/s, respectively, were obtained. The difference in the two values was due to the different viscosities of the solutions. A good fit of the experimental data was obtained which supports the use of the homogeneous model for this system. A counter-current ion exchange (CCIX) process was designed to treat nuclear waste at the Savannah River Site. A numerical method based on the orthogonal collocation method was used to simulate the concentration profile of cesium in the CCIX loaded with CST granules. To maximize cesium loading onto the CST and minimize the volume of CST, two design cases of a moving bed, where the fresh CST is pulsed into the column at certain periods or at certain concentration of cesium, were investigated. Simulation results showed that cesium removal behavior in the pilot-scale test of CCIX experiment, where the column length is 22 ft and the CST is pulsed 1 ft in every 24 hours, was well predicted by using the values of the effective diffusivities of 1.0 to 6.0 × 10-11 m2/s.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第19407号 / 工博第4123号 / 新制||工||1636(附属図書館) / 32432 / 京都大学大学院工学研究科合成・生物化学専攻 / (主査)教授 吉田 潤一, 教授 松田 建児, 教授 松原 誠二郎 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM