RESUMO
Nuclear-grade Spent Organic Resin (SOR) contains high concentrations of radioactive nuclides and metal contaminants, while phosphate sludge contains high amount of fine clayey particles and CO32-, both posing a major threat to the biosphere. In this study, a novel geopolymer package (GP) was proposed to directly solidify SOR loaded with 134Cs by incorporating uncalcined phosphate sludge (UPS) as feedstocks, activated by NaOH/KOH. The results showed that alkali-mixed reagents-activated GP is more advantageous in terms of chemical stability and mechanical properties than NaOH-activated GP, recording compressive strength values greater than the waste acceptance criteria and OPC. The 28-day compressive strength of solidified packages can exceed 31 MPa at the highest amount of 42 wt% UPS. The addition of NaF powder into the solidified packages generates more hybrid type gels, which are more conducive to partial dissolution and bonding UPS particles, thereby producing stable and stronger GP. Leaching results of solidified GP in presence of up to 13 wt% SORs showed that only 0.15 % of total 134Cs was leached, even under aggressive solutions. Solidification mechanism revealed that activation of UPS-MK blend forms N,K-A-S-H, (N,K,C)-A-S-H/C-S-H gels coexisting with unreacted particles, thereby solidify/stabilize metal contaminants and Cs+ by a synergetic immobilization action of hydration products via substitution and encapsulation. This study provides a promising paradigm for effective solidification of nuclear-grade resins and synergetic harmless treatment of industrial/phosphate mine solid wastes.