Adsorption and dissociation of Co-EDTA complexes in iron oxide-containing subsurface sands
- Pacific Northwest Lab., Richland, VA (United States)
- Univ. of Montana, Missoula, MT (United States)
The sorption of Co(II)EDTA{sup 2-} (where EDTA is ethylenediaminetetracetic acid) was investigated on goethite and on eight sand-textured Quaternary and Pliocene fluvial sediments. Dual-label tracer techniques were used to follow the distribution of {sup 60}Co(II)- {sup 14}C/EDTA added as the performed 1:1, Co(II) EDTA{sup 2-} complex. Sorption experiments were performed with fixed concentrations of Co(II)EDTA{sup 2-} (10{sup -5} mol/L) and variable pH (all materials), and fixed pH (4.4) with variable Co(II)EDTA{sup 2-} concentrations (two materials), using solids concentrations of 0.5 g/L for goethite and 500 g/L for the sediments and electrolyte concentrations of 0.003 and 0.03 (geothite only) mol/L Ca(ClO{sub 4}){sub 2}. Aqueous Fe{sub aq}{sup 3+} and Al{sub aq}{sup 3+} were measured at the time of the sorption determination. On goethite, Co(II)EDTA{sup 2-} exhibited anion-like sorption, increasing with decreasing pH. Increasing electrolyte concentration decreased sorption, indicating a weak, ion-pair type surface complex. Below pH 6, however, the sorption chemistry of Co{sup 2+} and EDTA{sup 4-} became complex and disparate as a result of Co(II)EDTA{sup 2-} dissociation. Dissociation was driven by exchange with Fe{sub aq}{sup 3+}. A nonelectrostatic surface complexation model that explicitly considered the Fe{sup 3+} -Co(II)EDTA{sup 2-} exchange reaction was able to adequately describe the sorption data using surface complexes with Co(II)EDTA{sup 2-}, FeEDTA{sup -}, and Co{sup 2+}. Iron oxides were a dominant grain-coating phase on over half the sorbents, and X-ray diffraction (XRD), chemical extraction, and microscopic techniques documented the presence of poorly crystalline forms as well as geothite, hematite, and feroxyhite. The coupled adsorption, dissolution, and dissociation process will cause complex distance-variant speciation and retardation behavior for Co(II)EDTA{sup 2-} in subsurface environments. 58 refs., 14 figs., 6 tabs.
- DOE Contract Number:
- AC06-76RL01830
- OSTI ID:
- 549037
- Journal Information:
- Geochimica et Cosmochimica Acta, Vol. 59, Issue 23; Other Information: PBD: 1995
- Country of Publication:
- United States
- Language:
- English
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