Effects of EDTA on the leaching behaviors of Cs(I) and Co(II) from cement waste forms

Abstract

Cementation is extensively employed for immobilizing radionuclides in low- and intermediate-level radioactive wastes generated during the decommissioning of nuclear power plants. Ethylenediaminetetraacetic acid (EDTA), used as a decontamination agent during the decommissioning process, can be introduced into the cement waste form containing radionuclides. This study investigated the effects of the EDTA present in simulated radioactive decommissioning wastes on the leaching behaviors of Co and Cs immobilized in the cement waste form. Co leaching was facilitated by the formation of highly mobile Co–EDTA complexes. However, Cs leaching was impeded by the competition for leaching with other metal–EDTA complexes. Moreover, the EDTA-induced carbonated layer with a dense pore structure played a crucial role as a retardation barrier for the Cs leaching. The calcite contents of the samples with 8 wt% EDTA were approximately three times higher than those of the samples without EDTA. The introduced EDTA affected the leaching behaviors of both Co and Cs, as well as the microstructure evolution of the cement waste form. Nevertheless, the addition of EDTA had a relatively low positive effect on the efficiency of Cs immobilization, but also an obvious negative effect on the efficiency of Co immobilization, regardless of the concentration of EDTA. Finally, an EDTA dosage of 1 wt% in the cement waste forms containing Co or Cs is suggested as a potential waste acceptance criterion for solidified low- and intermediate-level radioactive waste.