Effect of DTPA on europium sorption onto quartz - Batch sorption experiments and surface complexation modeling

Sorption of radionuclides on mineral surfaces retards their migration in the environment of a repository. Presence of organic ligands, however, affects sorption and consequently influences their transport behavior. In this study, we quantify the sorption of Eu(III) onto quartz surfaces as a function of pH in the absence and presence of diethylenetriaminepentaacetic acid (DTPA). Batch sorption experiments show a pH-dependent sorption of Eu(III) on quartz. The presence of DTPA results in slightly higher sorption of Eu(III) at neutral to slightly acidic pH and considerably lower sorption at alkaline conditions. Sorption experiments were simulated using the Diffuse Double Layer Model (DDLM) with single sorption sites (≡QOH) and monodentate surface complexation. The reactions were established based on the aqueous speciation calculation under the experimental conditions, and the thermodynamic constants of surface reactions were obtained and refined by numerical optimization. Results of surface complexation modeling show the formation of a surface species ≡QOHEuDTPA^2-, explaining the elevated sorption of Eu(III) at neutral to slightly acidic pH. In contrast, dissolved EuDTPA^2- complex species are present at alkaline pH, resulting in an enhanced mobility of Eu(III).