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Lead coprecipitation with iron oxyhydroxide nano-particles |
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| Authors: | Peng Lu Noel T Nuhfer Qin Li Hiromi Konishi Erika Elswick Chen Zhu |
| Institution: | a Department of Geological Sciences, Indiana University, Bloomington, IN 47405-1405, United States b Carnegie Mellon University, Department of Materials Sciences and Engineering, Pittsburgh, PA 15260, United States c Argonne National Laboratory, Biosciences Division, Argonne, IL 60439-4843, United States d State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210093, China e Department of Geoscience, University of Wisconsin-Madison, Madison, WI 53706, United States |
| Abstract: | Pb2+ and Fe3+ coprecipitation was studied with sorption edge measurements, desorption experiments, sorbent aging, High Resolution Transmission and Analytical Electron Microscopy (HR TEM-AEM), and geochemical modeling. Companion adsorption experiments were also conducted for comparison. The macroscopic chemical and near atomic scale HRTEM data supplemented our molecule scale analysis with EXAFS (Kelly et al., 2008). Coprecipitation of Pb2+ with ferric oxyhydroxides occurred at ∼pH 4 and is more efficient than adsorption in removing Pb2+ from aqueous solutions at similar sorbate/sorbent ratios and pH. X-ray Diffraction (XRD) shows peaks of lepidocrocite and two additional broad peaks similar to fine particles of 2-line ferrihydrite (2LFh). HRTEM of the Pb-Fe coprecipitates shows a mixture of 2-6 nm diameter spheres and 8-20 by 200-300 nm needles, both uniformly distributed with Pb2+. Geochemical modeling shows that surface complexation models fit the experimental data of low Pb:Fe ratios when a high site density is used. Desorption experiments show that more Pb2+ was released from loaded sorbents collected from adsorption experiments than from Pb to Fe coprecipitates at dilute EDTA concentrations. Desorbed Pb2+ versus dissolved Fe3+ data show a linear relationship for coprecipitation (CPT) desorption experiments but a parabolic relationship for adsorption (ADS) experiments.Based on these results, we hypothesize that Pb2+ was first adsorbed onto the nanometer-sized, metastable, iron oxyhydroxide polymers of 2LFh with domain size of 2-3 nm. As these nano-particles assembled into larger particles, some Pb2+ was trapped in the iron oxyhydroxide structure and re-arranged to form solid solutions. Therefore, the CPT contact method produced more efficient removal of Pb2+ than the adsorption contact method, and Pb2+ bound in CPT solids represent a more stable sequestration of Pb2+ in the environment than Pb2+ adsorbed on iron oxyhydroxide surfaces. |
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