Remediation by waste marble powder and lime of jarosite-rich sediments from Portman Bay (Spain)

We investigate the use of hydrated lime and calcite waste marble powder as remediation treatments of contaminated jarosite-rich sediments from Portman Bay (SE, Spain), one of the most contaminated points in the Mediterranean coast by mining-metallurgical activities. We tested two commercial hydrated limes with different Ca(OH)₂ percentages (28 and 60% for Lime-1 and Lime-2 respectively) and two different waste marble powder, WMP, from the marble industry (60 and 96% of calcite for WMP-1 and WMP-2 respectively). Mixture and column experiments and modelling of geochemical reactions using PHREEQC were performed. Lime caused the precipitation of hematite, gypsum and calcite, whereas WMP treatments formed iron carbonates and hematite. The fraction of amorphous phases was mainly composed of iron oxides, hydroxides and oxyhydroxides that was notably higher in the lime treatment in comparison to the WMP treatment. The reactive surface area showed a positive trend with the amorphous phase concentration. Results highlighted the effectiveness of lime treatments, where Lime-2 showed a complete elimination of jarosite. Column experiments revealed a clear reduction of heavy metal concentration in the lixiviate for the treated sediments compared to the original sediments. Particularly, Lime-2 showed the highest reduction in the peak concentration of Fe, Mn, Zn and Cd. The studied treatments limited the stabilisation of Cr and Ni, whereas contrarily As increases in the treated sediment. PHREEQC calculations showed that the most concentrated heavy metals (Zn and Mn) are stabilized mainly by precipitation whereas Cu, Pb and Cd by a combination of precipitation and sorption processes. This chemical environment leads to the precipitation of stable iron phases, which sorb and co-precipitate considerable amounts of potentially toxic elements. Lime is significantly more effective than WMP, although it is recommended that the pH value of the mixture should remain below 9 due to the amphoteric behaviour of heavy metals.