Mobility of radionuclides (RNs) in natural water systems can be increased by complex formation with organic materials. In alkaline cement pore-water conditions, cellulose materials in radwastes such as woods and papers are degraded fast to small organic materials. As a major cellulose degradation product, isosaccharinate (ISA) has been paid attention recently due to its effect on facilitating RNs migration. ISA contains a carboxyl and four hydroxyl functional groups, which cooperatively interact to form chelating bonds with positively charged radionuclides. In our previous study, we determined thermodynamic formation constants, reaction enthalpy and entropy of trivalent americium complexes with ISA, Am(ISA)n (3-n)+ (n=1, 2), in weak acidic condition by conducting temperature-dependent UVVis absorption spectroscopy. Based on those thermodynamic constants along with the experimental results from time-resolved laser induced fluorescence spectroscopy and DFT calculations, we suggested two different chelating-modes of ISA on Am(III). It is more relevant to study Am(III)-ISA complexation under alkaline conditions around pH 12.5, which correspond to the pore-water condition of calciumsilicate- hydrate. Under the alkaline conditions, deprotonated hydroxyl groups of ISA can form more strong interactions with Am. Aquatic hydroxide group can also act as a ligand to form ternary Am(III) -ISA-OH complexes. In this study, absorption spectra of Am-ISA systems were monitored with two variations: first, pH variation (5.5–13) in the presence of constant 30 mM ISA, and second, ISA concentration variation (20 μM – 30 mM) at constant pH of 12.5. As increasing the pH at constant 30 mM ISA, absorption spectra of Am(ISA)2 + were red-shifted from 506.3 to 509.5 nm. The samples showed stable absorption spectra over 30 days. On the other hand, samples with lower ISA concentrations below 10 mM at pH 12.5, showed gradual decrease in the absorbance as sample aging time. By examining filtrates after ultrafiltration (1 kDa), we confirmed that aqueous Am(III)-ISA complexes were formed in the presence of 30 mM ISA at pH 12.5, while colloidal particles and precipitations were formed in the conditions of ISA concentrations lower than 10 mM. In this presentation, we will discuss about probable ternary complex forms of Am(III)-ISA-OH, colloidal forms, and solubility of Am(III) as a function of ISA concentration under alkaline conditions. Absorption and luminescence spectroscopic properties of the Am(III)-ISA-OH ternary system will also be presented.

• Hee-Kyung Kim(Korea Atomic Energy Research Institute (KAERI)) Corresponding author
• Hye-Ryun Cho(Korea Atomic Energy Research Institute (KAERI))