Arsenic contamination in abandoned and active gold mine spoils in Ghana: Geochemical fractionation, speciation, and assessment of the potential human health risk

This work aims to study the pseudo-total content, geochemical fractions, and species of arsenic (As) in the bulk soil and in the coarse and fine particles of top soil and soil profiles collected from active and abandoned gold mine spoils in Ghana. The human health risk for adults (male and female) and children has been assessed. To achieve our aims, we collected 51 samples, characterized them, determined the total As content, and sequentially extracted the geochemical fractions of As including water-soluble and un-specifically bound As (FI); specific-sorbed/exchangeable As (FII); poorly (FIII)- and well-crystalline (IV) Fe oxide; and residual/sulphide fraction (FV). In selected samples, As species were determined using synchrotron-based X-ray absorption near edge structure (XANES). Pseudo-total As contents varied from 1807 to 8400 mg kg⁻¹, with the extremes occurring at the abandoned mine spoil. Arsenic was almost 10-fold higher in the fine particles (<0.63 μm) than in the coarse particles. Arsenic was mainly associated with FIII and FV, indicating that the distribution of As in these spoils is governed by their contents of amorphous Fe oxides, sulphides and As bearing minerals. The XANES results indicated that scorodite (FeAsSO₄ = 65–76%) and arsenopyrite (FeAsS = 24–35%) are the two major As-containing minerals in the spoils. The potential mobility (PMF = ∑FI-FIV) of As in the fine particles of the top soil was higher (48–61%) than in the coarse particles (25–44%). The mobile fraction (MF) (FI+FII) and PMF of As in the coarse particles of the profiles increased with depth while it decreased in the fine particles. The median hazard index values indicated an elevated human health risk, especially for children. The high contamination degree and potential mobility of As at the studied mine spoils indicate high potential risk for human and environmental health.