Abstract

Wastes from a former Portuguese steel plant were deposited between 1961 and 2001 on the riverbank of a tributary of the Tagus River creating a landfill connected to the river, posing a potential contamination risk to the Tagus estuary ecosystem. This study aims to assess the transfer of chemical elements from contaminated sediments to the estuarine water from cycles of sediment leaching so as to evaluate the ecotoxicity of the leachates, and to analyze the solid phases crystallized from those leachates. Landfill sediment and estuarine water samples were collected during low tide. Sediment samples were analyzed for pH, electric conductivity (EC), Corg, NPK, and iron oxides. Leaching assays (four replicates) were done using estuarine water (200 cm3/replicate) and 1.5 kg of sediment per reactor. Each reactor was submitted to four leaching processes (0, 28, 49, and 77 days). The sediment was kept moist between leaching processes. Sediment (total (acid digestion) and available fraction (diluted organic acid extraction-Rhizo)) elemental concentrations were determined by inductively coupled plasma–instrumental neutron activation analysis (ICP/INAA). Leachates, and estuarine and sediment pore waters were analyzed for metals/metalloids by ICP/mass spectrometry (MS) and carbonates/sulfate/chloride by standard methodologies. Ecotoxicity assays were performed in leachates and estuarine and pore waters using Artemia franciscana and Brachionus plicatillis. Aliquots of the leachates were evaporated to complete dryness (23–25 °C) and crystals analyzed by X-ray powder diffraction (XRD). Sediment with pH = 8 and high EC and Corg was contaminated with As, Cd, Cr, Cu, Pb, and Zn. The element concentrations in the available fraction of the sediment were low compared to the sediment total concentrations (<1 % for Rhizo extraction). The concentrations of potentially hazardous elements in the estuarine water were relatively low, except for Cd. Concentrations of hazardous elements in the leachates were very low. Calcium, K, Mg, Na, and chloride concentrations were high but did not vary significantly among the four leaching experiments. Total concentrations of carbonate were much higher in leachates than in estuarine water. Both estuarine water and leachates showed negligible toxicity. Crystals identified in the solids obtained from the leachates by evaporation were halite, anhydrite, epsomite, dolomite, and polyhalite. The sediment showed the capacity to retain the majority of the potentially hazardous chemical elements. Remobilization of chemical elements from sediment by leaching was essentially negligible. The variation of total concentrations of Ca, carbonate, and sulfate in leachates indicates that the sediment contained reactive sulfides. Due to its composition, the sediment seems to be a dynamic system of pollution control, which should not be disturbed.

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