Nonlinear cesium release behavior from idiomorphic analcime–pollucite solid solutions with controlled cesium content
摘要
Analcime–pollucite solid solutions (APSS) are among the most promising host materials for radioactive Cs immobilization. However, reported Cs release behaviors differ substantially across the literature because key physicochemical properties have not been systematically controlled. Here, we synthesized idiomorphic APSS with controlled Cs contents to minimize morphological heterogeneity and evaluate intrinsic Cs release behavior. Using this approach, we identified two key phenomena governing Cs release. First, crystal size decreases once the Cs content exceeds 17.302 wt% and declines further with increasing Cs content. Second, APSS spontaneously develops a self-organized core–rim structure consisting of a Cs-enriched core and a Na-enriched rim that suppresses Cs release, consistent with the preservation of Cs-rich cores in natural pollucite over geological timescales. Together, these competing effects produce a nonlinear relationship between Cs content and Cs release, demonstrating that radionuclide release from host materials cannot be assumed to be linearly proportional to radionuclide content.