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Characterization of Nano-scale Aluminum Oxide Transport Through Porous MediaNorwood, Sasha Norien 01 January 2013 (has links)
Land application of biosolids has become common practice in the United States as an alternative to industrial fertilizers. Although nutrient rich, biosolids have been found to contain high concentrations of emerging contaminants (e.g. pharmaceuticals, personal care products) while containing a significant fraction of inorganic nano-scale colloidal materials such as oxides of iron, titanium, and aluminum.
Given their reactivity and small size, there are many questions concerning the potential migration of these nano-sized colloidal materials through the soil column and into our surface and groundwater bodies. Transport of emerging pollutants of concern through the soil column, at minimum, is impacted by colloidal properties (e.g. chemical composition, shape, aggregation kinetics), solution chemistry (e.g. pH, ionic strength, natural organic matter), and water flow velocity. The purpose of this current research was to characterize the long-term transport behavior of aluminum oxide nanoparticles (Al2O3) through a natural porous media with changes in pH, aqueous-phase concentration, pore-water velocity and electrolyte valence. Additionally, deposition rates during the initial stages of deposition were compared to several models developed based on colloid filtration theory and DLVO stability theory. Benchtop column laboratory experiments showed that, under environmentally relevant groundwater conditions, Al2O3 nanoparticles are mobile through saturated porous media. Mobility increased under conditions in which the nanoparticles and porous media were of like charge (pH 9). Changes in linear pore water velocity, under these same high pH conditions, showed similar transport behavior with little mass retained in the system. Deposition is believed to be kinetically controlled at pH 9, as evidenced by the slightly earlier breakthrough as flow rate increased and was further supported by observed concentration effects on the arrival wave following several stop flows.
While lower aqueous-phase concentrations resulted in significantly longer breakthrough times, the total mass retained in the system was found to be independent of concentration. Additionally, experimental deposition rate coefficients (kd), used to describe deposition kinetics under "clean bed" conditions, were similar across the aqueous-phase concentrations studied. The use of calcium chloride electrolyte solution in transport studies resulted in enhanced mobility relative to potassium chloride suggesting that changes in groundwater solution chemistry could impact mobility of contaminants associated with biosolids. Predicted deposition rate coefficients, using three different models, were found to under- or over-predict values relative to those experimentally determined values depending on the model. This current research has shown that nanocolloids associated with biosolids, specifically Al2O3, are mobile through saturated porous media. Given the ubiquity of nanocolloidal materials, particularly engineered nanomaterials, coupled with the expected increase in land-application of biosolids, a clear understanding of their transport and fate is prudent to understanding the potential impact these emerging pollutants may have on our surface and groundwater bodies.
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