Abstract

Understanding the fate and transport of radionuclides in porous media reduces the risk of contaminating soils and groundwater systems. While the cotransport of bentonite colloids (BC) with radionuclides in saturated media is well documented, the role of phosphate (P) in the colloid-driven transport of radionuclides in saturated porous media is still unaddressed; in particular, phosphate increases the mobilities of radionuclides in porous media, which should be subjected to an environmental risk assessment and model construction. In this work, the effects of phosphate on the transport and release of Eu(III) in different colloid systems (P-Eu(III), P-BC, P-BC-Eu(III)) was investigated with a fundamental colloid chemistry approach and a range of characterization techniques. The results showed that intrinsic europium colloids with size of 685 nm were formed by precipitation with phosphate, which affected the mobility of Eu(III) due to colloid stability and physical straining. Phosphate enhanced BC and BC-Eu(III) transport, and a high phosphate concentration promoted BC transport by eliminating physical straining and enhancing the electrostatic repulsions. The crystal structure of EuPO4 was not destroyed by the subsequent introduction of BC, which carried EuPO4 for further migration. However, when phosphate, bentonite and Eu(III) coexisted in a colloid suspension, the phosphate promoted Eu(III) transport by preferentially interacting with the BC to form ternary BC-P-Eu(III) pseudo-colloids rather than forming the intrinsic EuPO4 colloids. The synergetic role of P and BC on Eu(III) transport involved a relatively complex process and was not a simply additive effect. The findings in this work highlight the significance of phosphate in controlling the fate and transport of Ln(III)/Am(III) radionuclides in the presence of intrinsic colloids and pseudo-colloids in P-rich colloid-bearing environments.

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