title: Simulation of the mobility of metal-EDTA complexes in groundwater: the influence of contaminant metals.
abstract: Reactive transport simulations were conducted to model chemical reactions between metal-EDTA (ethylenediaminetetraacetic acid) complexes during transport in a mildly acidic quartz-sand aquifer. Simulations were compared with the results of small-scale tracer tests wherein nickel-, zinc-, and calcium-EDTA complexes and free EDTA were injected into three distinct chemical zones of a plume of sewage-contaminated groundwater. One zone had a large mass of adsorbed, sewage-derived zinc; one zone had a large mass of adsorbed manganese resulting from mildly reducing conditions created by the sewage plume; and one zone had significantly less adsorbed manganese and negligible zinc background. The chemical model assumed that the dissolution of iron(III) from metal-hydroxypolymer coatings on the aquifer sediments by the metal-EDTA complexes was kinetically restricted. All other reactions, including metal-EDTA complexation, zinc and manganese adsorption, and aluminum hydroxide dissolution were assumed to reach equilibrium on the time scale of transport; equilibrium constants were either taken from the literature or determined independently in the laboratory. A single iron(III) dissolution rate constant was used to fit the breakthrough curves observed in the zone with negligible zinc background. Simulation results agreed well with the experimental data in all three zones, which included temporal moments derived from breakthrough curves at different distances downgradient from the injections and spatial moments calculated from synoptic samplings conducted at different times. Results show that the tracer cloud was near equilibrium with respect to Fe in the sediment after 11 m of transport in the Zn-contaminated region but remained far from equilibrium in the other two zones. Sensitivity studies showed that the relative rate of iron(III) dissolution by the different metal-EDTA complexes was less important than the fact that these reactions are rate controlled. Results suggest that the published solubility for ferrihydrite reasonably approximates the Fe solubility of the hydroxypolymer coatings on the sediments. Aluminum may be somewhat more soluble than represented by the equilibrium constant for gibbsite, and its dissolution may be rate controlled when reacting with Ca-EDTA complexes.
authors.affiliation: School of Chemical Engineering Practice, Massachusetts Institute of Technology, Cambridge 02139, USA.
authors.forename: J C
authors.initials: JC
authors.lastname: Friedly
authors.forename: D B
authors.initials: DB
authors.lastname: Kent
authors.forename: J A
authors.initials: JA
authors.lastname: Davis
mesh_terms: D002614:Chelating Agents / Q000737:chemistry*; D004492:Edetic Acid / Q000737:chemistry*; D007700:Kinetics; D019216:Metals, Heavy / Q000737:chemistry*; D008962:Models, Theoretical; D012989:Soil Pollutants / Q000032:analysis*; D012995:Solubility; D014873:Water Pollutants / Q000032:analysis*
chemical_list: D002614:Chelating Agents; D019216:Metals, Heavy; D012989:Soil Pollutants; D014873:Water Pollutants; D004492:Edetic Acid