『Abstract
Lead- and Pb-As-jarosites are minerals common to acidic, sulphate-rich
environments, including weathering zones of sulphide ore deposits
and acid rock or acid mine drainage (ARD/AMD) sites, and often
form on or near galena. The structures of these jarosites are
based on linear tetrahedral-octahedral-tetrahedral (T-O-T) sheets,
comprised of slightly distorted FeO6 octahedra
and SO42- (-AsO43-
in Pb-As-jarosites) tetrahedra. To better understand the dissolution
mechanisms and products of the break down of Pb- and Pb-As-jarosite,
preliminary batch dissolution experiments were conducted on synthetic
Pb- and Pb-As-jarosite at pH 2 and 20℃, to mimic environments
affected by ARD/AMD, and at pH 8 and 20℃, to simulate ARD/AMD
environments recently remediated with slaked lime (Ca(OH)2). All four dissolutions are incongruent. Dissolution
of Pb-jarosite at pH 2 yields aqueous Pb, Fe and SO42-.
The pH 8 Pb-jarosite dissolution yields aqueous Pb, SO42-
and poorly crystalline Fe(OH)3, which does
not appear to resorb Pb or SO42-,
possibly due to the low solution pH (3.44-3.54) at the end of
the experiment. The pH 2 and 8 dissolutions of Pb-As-jarosite
result in the formation of secondary compounds (poorly crystalline
PbSO4 for pH 2 dissolution; poorly crystalline
PbSO4 and Fe(OH)3 for
pH 8 dissolution), which may act as dissolution inhibitors after
250 to 300 h of dissolution. In the pH 2 dissolution, aqueous
Fe, SO42- and AsO43-
also form, and in the pH 8 dissolution, Fe(OH)3
precipitates then subsequently resorbs aqueous AsO43-. The dissolutions probably proceed
by preferred dissolution of the A- and T-sites, which contain
Pb, and SO42- and AsO43-,
respectively, rather than Fe, which is sterically remote, within
the T-O-T Pb- and Pb-As-jarosite structures. These data provide
the foundation necessary for further, more detailed investigations
into the dissolution of Pb- and Pb-As-jarosites.
Keywords: Pb-jarosite; Pb-As-jarosite; Fe hydroxide; Pb sulphate;
acid mine drainage; dissolution』
1. Introduction
2. Methods and materials
2.1. Synthesis of Pb- and Pb-As-jarosites
2.2. Characterization of synthetic Pb- and Pb-As-jarosites
2.3. Dissolution experiments
3. Results
3.1. Characterization of synthetic Pb- and Pb-As-jarosites
3.2. Dissolution at pH 2
3.2.1. Solution chemistry
3.2.2. Residual solids
3.3. Dissolution at pH 8
3.3.1. Solution composition
3.3.2. Residual solids
4. Discussion
4.1. Pb-jarosite
4.1.1. Dissolution at pH 2
4.1.2. Dissolution at pH 8
4.2. Pb-As-jarosite
4.2.1. Dissolution at pH 2
4.2.2. Dissolution at pH 8
4.3. Comparison of Pb-jarosite and Pb-As-jarosite dissolutions,
and environmental implications
5. Conclusions
Acknowledgements
References