Geochemical stability of potentially toxic elements in porphyry copper-mine tailings from Chile as linked to ecological and human health risks assessment

The geochemical stability, in terms of potential mobility and derived ecological and human health risks of potentially toxic elements (PTEs), of diverse fresh and old porphyry Cu-mine tailings from Chile was assessed through an integrated methodology comprising four interrelated investigation levels: (1) chemical composition and contamination degree of tailings by PTEs, (2) mineralogical characterization by X-ray diffraction and quantitative automated mineralogy analysis by scanning electron microscopy (QEMSCAN(R)), (3) partitioning and potential mobility of PTEs within the tailings by a sequential extraction procedure (SEP) and leaching tests, and (4) ecological risk assessment (ERA) and human health risk assessment (HHRA). According to pollution indices, Cu, As, Pb, and Mo are most concerning PTEs present in the tailings. SEP shows that major portion of the PTEs are strongly fixed as residual fraction, and thus are poorly mobilizable and bioavailable. Among the PTEs, Cu, As, and Mo were identified as the PTEs most prone to mobilization. Leaching tests show that a low fraction of PTEs is water-leachable. Seawater enhances Mn and As leaching, while process water increases the leaching of Cu, Mn, and Mo. Phosphate particularly promotes leaching of As and Cu, whereas it does not mobilize or even immobilize Pb in the tailings. ERA suggests that mainly old tailings pose a very high potential risk for ecological receptors (PERI = 663-3356), mostly due to Cu and As. HHRA indicates that the old tailings pose higher potential non-carcinogenic and carcinogenic health risks, while the risk decreases in the order ingestion > dermal > inhalation for both children and adults. Non carcinogenic and carcinogenic HHRA points to As as the main PTE of concern via ingestion pathway in the tailings. Overall, the results revealed that particularly old tailings, containing mixed slag-tailings, pose considerable risks to the environment and human health due to potential PTEs mobilization and this aspect requires scrutiny for proper tailings management, including storage, sealing, and eventual tailings reprocessing and/or site rehabilitation after closure.