The adsorption of Eu(III) and Am(III) on Beishan granite: XPS, EPMA, batch and modeling study

Abstract

Granite has been chosen as a promising host rock for geological repository of high-level radioactive waste in many countries. However, the description of radionuclide adsorption on granite is subjected to its complicated composition and still a challenge. We studied the adsorption of Eu(III) and Am(III) on Beishan granite, a preliminary selection of host rock in China, as a function of pH, adsorbate concentration, ionic strength and the composition of background electrolytes. A surface complexation model was set up using Generalized Composite approach based on Eu(III) adsorption in NaCl electrolyte, supported by X-ray photoelectron spectroscopy and verified by Eu(III) adsorption in the presence of CO2 at PCO2=10-3.58atm and in CaCl2 electrolyte. The model was successfully extended to describe Am(III) adsorption in both NaCl and CaCl2 electrolytes. It was also found that temperature effect on Eu(III) adsorption was negligible at 25–80°C, that the adsorption of Eu(III) on freshly crushed granite with “new” surfaces and aged granite with “old” surfaces were identical to each other, and that the presence of fulvic acid of 2–20mg/L significantly declined the distribution coefficients of Eu(III) and Am(III) in high pH range. Electron probe micro analyses indicated that biotite had higher affinity for Eu(III) than other major minerals, such as oligoclase, quartz and orthoclase.