Journal
CHEMICAL GEOLOGY
Volume 372, Issue -, Pages 109-118Publisher
ELSEVIER
DOI: 10.1016/j.chemgeo.2014.02.019
Keywords
Iron(II); Humic substances; Complexation; Sorption; PHREEQC-Model VI; PHREEPLOT
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The complexation of Fe(II) with organic matter (OM) and especially with humic acids (HAs) remains poorly characterized in the literature. In this study, batch experiments were conducted on a pH range varying from 1.95 to 9.90 to study HA-mediated Fe(II) binding. The results showed that high amounts of Fe(II) are complexed with HA depending on the pH. Experimental data were used to determine a new set of binding parameters by coupling PHREEPLOT and PHREEQC-Model VI. The new binding parameters (log K-MA = 2.19 +/- 0.16, log K-MB= 4.46 +/- 0.47 and Delta LK2 = 3.90 +/- 1.30) were validated using the LFER (linear free energy relationship) method and published adsorption data between Fe(II) and Suwannee River fulvic acid (SRFA) (Rose andWaite, 2003). They were then put in PHREEQC-Model VI to determine the distribution of Fe(II) onto HA functional groups. It was shown that Fe(II) forms mainly bidentate complexes, some tridentate complexes and only a few monodentate complexes with HA. Moreover, Fe(II) is mainly adsorbed onto carboxylic groups at acidic and neutral pH, whereas carboxy-phenolic and phenolic groups play a major role at basic pH. The major species adsorbed onto HA functional groups is Fe2+; Fe(OH)(+) appears at basic pH (frompH 8.13 to 9.9). The occurrence of OM and the resulting HA-mediated binding of Fe(II) can therefore influence Fe(II) speciation and bioavailability in peatlands and wetlands, where seasonal anaerobic conditions prevail. Furthermore, the formation of a cationic bridge and/or the dissolution of Fe(III)-(oxy) hydroxides by the formation of Fe(II)-OM complexes can influence the speciation of other trace metals and contaminants such as As. (C) 2014 Elsevier B.V. All rights reserved.
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