A multi-scale assessment of Pb(II) sorption on dolomite

Macroscopic sorption studies indicated that Pb sorption capacity was independent of pH over the pH range 5–7, while sorption as a function of reaction time up to two weeks for systems with no bulk precipitate phases showed continuous Pb uptake on dolomite. This could be due to diffusion of Pb into the micropores of dolomite as well as an increase in surface sites caused by particle size reduction during suspension mixing. Normalized XANES spectra for systems undersaturated with respect to Pb carbonate precipitates resembled the spectrum of Pb4(OH)4+4, suggesting that Pb is mainly coordinated to dolomite as an inner-sphere surface complex. On the other hand, the XANES spectrum for 10−3 M Pb at 1 atm CO2(g) in a 2 M Mg(NO3)2 background electrolyte solution resembled that of cerussite, while a sample at 5×10−4 M Pb5×10−4 M Pb in equilibrium with air and 2 M Mg(NO3)2 resembled that of hydrocerussite. EXAFS analyses of sorption samples in chloride solutions showed that there were only first-shell contributions under 1 atm CO2(g), while higher shell contributions from Ca/Mg were seen at 10−3.42 atm CO2(g). On the other hand, EXAFS samples prepared in nitrate solutions showed noticeable differences in speciation under different reaction conditions—from outer-sphere surface complexes at low Pb concentrations and pH, to inner-sphere surface complexes at moderate Pb concentrations and neutral pH, to the formation of Pb carbonate precipitates at the highest Pb loadings.

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