PNNL

Abstract

Hydroxyapatite nanoparticle (nHAP) is being used to remediate soils and aquifers contaminated with metals and radionuclides; however, the mobility of nHAP is still poorly understood in subsurface granular environments. In this study, transport and retention kinetics of alizarin red S (ARS)-labeled nHAP were investigated in water-saturated quartz sand at low concentrations of surfactants: sodium dodecyl benzene sulfonate (SDBS, an anionic surfactant, 0–50 mg L–1) and cetyltrimethylammonium bromide (CTAB, a cationic surfactant, 0–5 mg L–1). Both surfactants were found to have a marked effect on the electrokinetic properties of ARS-nHAP and, consequently, on their transport and retention behaviors. Transport of nanoparticles (NPs) increased significantly with increasing SDBS concentration, largely because of enhanced colloidal stability and reduced aggregate size arising from enhanced electrostatic, osmotic, and elastic-steric repulsions between ARS-nHAP and sand grains. Conversely, transport decreased significantly in the presence of increasing CTAB concentrations due to reduced surface charge and consequential enhanced aggregation of the NPs. Osmotic and elastic-steric repulsions played only a minor role in enhancing the colloidal stability of ARS-nHAP in the presence of CTAB. Retention profiles of ARS-nHAP exhibited hyperexponential-shapes (decreasing rates of retention with increasing distance) for all conditions tested, and became more pronounced as CTAB concentration increased. The phenomenon was attributed to the aggregation and ripening of ARS-nHAP in the presence of surfactants, particularly CTAB. Overall, the present study suggests that surfactants at environmentally relevant concentrations may be an important consideration in employing nHAP for engineered in-situ remediation of certain metals and radionuclides in contaminated soils and aquifers.