Influences of pH and residence time on Pb(II) retention in calcitic systems

GEOC 41

Ashaki A. Rouff1, Richard J. Reeder1, and Nicholas S. Fisher2. (1) Department of Geosciences and Center for Environmental Molecular Science, SUNY at Stony Brook, Stony Brook, NY 11794-2100, (2) Marine Sciences Research Center and Center for Environmental Molecular Science, SUNY at Stony Brook, Stony Brook, NY 11794-5000
Pb(II) sorption experiments with calcite powders were conducted at ambient pressure and temperature over a pH range of 6.9-9.4. The pH sorption edge correlates well with PbCO30(aq) speciation, alluding to the influence of this metal complex on Pb-calcite interaction. Desorption experiments at pH 7.4, 8.3 and 9.4 demonstrate a subtle residence time effect on metal uptake. Hysteresis is slight at pH £ 8.3, but becomes pronounced at pH 9.4, suggesting the presence of significant irreversibly bound Pb at high pH. Linear combination fits of X-ray absorption near edge spectra for samples sorbed at pH 9.4 confirm an adsorbed component (80%) and non-exchangeable fraction (20%) as co-precipitated Pb. We propose that incorporation occurs as a result of high calcite re-crystallization rates at pH > 8.3. This study highlights the role of aqueous metal complexation on initial Pb uptake, and demonstrates the role of pH in Pb immobilization in calcitic systems.