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DIVISION S-2-SOIL CHEMISTRY

Adsorption of Mercury(II) by Variable Charge Surfaces of Quartz and Gibbsite

^a Soil and Water Sci. Dep., Univ. of Florida, Gainesville, FL, 32611-0290 USA
^b Dep. of Plant and Soil Sci., The Univ. of Tennessee, Knoxville, TN 37901-1071 USA
^c Dep. of Geological Sci., The Univ. of Tennessee, Knoxville, TN 37996-1410 USA

messington{at}utk.edu

The influence of pH, ionic strength, ligands (Cl, SO₄, PO₄), and metals (Ni and Pb) on the adsorption of Hg(II) by quartz and gibbsite was investigated to better understand the Hg(II) adsorption process and the impact of metals and ligands on this process. The triple layer model (TLM) was used to simulate Hg(II) adsorption on both surfaces. Mercury(II) adsorption from a 0.6 µM Hg(II) solution varies as a function of pH, increasing to an adsorption maximum with increasing pH before tailing off to a constant level at high pH values. The pH at which maximum Hg(II) adsorption occurs (pH_max 4.5) is comparable to the pK_a (3.2) for the hydrolysis of Hg²⁺ to form Hg⁰₂. Further, the Hg(II) adsorption edge shifts to much higher pH values in the presence of 0.001 M and 0.01 M Cl, which also corresponds to the pH at which Hg⁰₂ is predicted to form. Only minor deviations in the degree of adsorption and the shape of the Hg(II) adsorption edge are influenced by ionic strength, suggesting the formation of inner-sphere surface complexes. However, Hg(II) adsorption can only be successfully modeled with consideration of the formation of both an outer-sphere surface complex [XO^-–HgOH⁺] and an inner-sphere surface complex [XOHg^-₂]. Swamping concentrations (0.01 M) of SO₄ and PO₄ reduced Hg(II) adsorption on quartz, a result of the predicted formation of Hg(OH)₂SO^2-₄, Hg(OH)₂H₂PO^-₄, and Hg(OH)₂–HPO^2-₄ aqueous species (the adsorption edge and pH_max were not influenced). The presence of SO₄ also decreased Hg(II) retention by gibbsite, which was also attributed to the formation of the Hg(OH)₂SO^2-₄ ion pair; however, the presence of PO₄ increased Hg(II) retention by gibbsite, which was attributed to the formation of a phosphate bridge [AlOPO₃Hg^2-₂]. Mercury(II) adsorption was decreased in the presence of 14 µM Pb and 48 µM Ni, and most noticeably in the quartz system. The adsorption of Hg(II), when in competition with Pb or Ni, could not be simulated by the TLM without the reoptimization of the Hg(II) outer- and inner-sphere log K_int values. Intrinsic Hg(II) adsorption constants derived from single-element systems could not be employed to simulate adsorption in multi-element, competitive systems.

Abbreviations: IS, ionic strength • TLM, triple layer model

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