Determination of contamination sources and geochemical behaviors of metals in soil of a mine area using Cu, Pb, Zn, and S isotopes and positive matrix factorization

The use of multiple isotopic ratios and statistical methods can substantially increase the reliability and precision of determining contamination sources and pathways. In this study, contamination sources were differentiated in three subareas in one mine area and geochemical processes were investigated using Cu, Pb, Zn, and S isotopes and positive matrix factorization (PMF). Soil samples downstream of the adit seepages exhibited distinctly higher δ65Cu values than those from other areas. δ65Cu in adit seepages increased substantially from ore sulfides owing to large isotopic fractionation during oxidative dissolution. Although δ65Cu decreased during sulfide precipitation in seepage-contaminated soil, the discrimination of δ65Cu was still valid. Therefore, δ65Cu is particularly useful for differentiating between contamination by sulfides (tailings) and water (adit seepages). Moreover, sulfide precipitation following sulfate reduction was verified by the decreased δ66Zn and δ34S in the soil. In addition, the plot of 208Pb/206Pb versus Pb-1 distinguished contamination sources. Furthermore, PMF analysis confirmed the determination of sources and differentiated between contamination by As- and Cu-enriched tailings. The effect of Cu-enriched tailings further downstream suggested that the lower specific gravity of chalcopyrite compared to that of arsenopyrite affected the distribution of soil contamination. [Display omitted] •High and low δ65Cu indicated water and sulfide contamination sources, respectively.•Cu, Zn, and S isotopes elucidated contaminants precipitated as sulfides in an area.•δ65Cu and δ66Zn were higher in partial dissolution than total extraction.•Pb isotopes could differentiate between soil contamination by water and tailings.•PMF could differentiate between contamination by As- and Cu-enriched tailings.