Groundwater remediation using iron oxide and zero-valent iron nanoparticles (NPs) can be effective, but is limited in many applications due to the NP strong retention in groundwater-saturated porous media after injection, the passivation of the porous surface, and the high cost of nanomaterials versus macro scale iron. In this study, we investigated transport of bare and polymer-coated 2-line ferrihydrite NPs (30–300 nm) in saturated aquifer sediments. The influence of poly(acrylic acid) (PAA) polymer coatings was studied on the colloidal stability and transport in sediments packed column tests simulating groundwater flow in saturated sediments. In addition, the influence of calcium cations was investigated by transport measurements using sediments with calcium concentrations in the aqueous phase ranging from 0.5 (typical for most sediments) to 2 mM. Measurements were also made of zeta potential, hydrodynamic diameter, polymer adsorption and desorption properties, and bio-availability of PAA-coated NPs. We found that NP transport through the saturated aquifer sediments was improved by PAA coating and that the transport properties could be tuned by adjusting the polymer concentration. We further discovered that PAA coatings enhanced NP transport, compared to bare NPs, in all calcium-containing experiments tested, however, the presence of calcium always exhibited a negative effect on NP transport. In tests of bioavailability, the iron reduction rate of the coated and bare NPs by Geobacter sulfurreducens was the same, which shows that the PAA coating does not significantly reduce NP Fe(III) bioavailability. Our results demonstrate that much improved transport of iron oxide NP can be achieved in saturated aquifer sediments by introducing negatively charged polyelectrolytes and optimizing polymer concentrations, and furthermore, these coated NPs retain their bioavailability that is needed for applications in bio-environmental remediation.
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The authors acknowledge support of the Andlinger Innovation Fund of the Andlinger Center for Energy and the Environment at Princeton University. The authors thank Prof. Robert Prud’homme for his valuable discussions and his group for assistance.
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Desorption dynamics of PAA from 2-line ferrihydrite NP surfaces in a dilute solution
Data shown in Fig. 4 were used to determine a desorption rate of 47.73 mg PPA/g NP/h for 8 mg/l PAA-coated 2-line ferrihydrite NPs in an infinitely dilute solution containing a carbonate/bicarbonate buffer at pH 8. This demonstrates that PAA will detach from the NPs and be lost into the groundwater when the coated NPs are contacted with fresh groundwater.
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Xiang, A., Zhou, S., Koel, B.E. et al. Transport of poly(acrylic acid) coated 2-line ferrihydrite nanoparticles in saturated aquifer sediments for environmental remediation. J Nanopart Res 16, 2294 (2014). https://doi.org/10.1007/s11051-014-2294-5