Physiochemical controls on the formation and stability of atacamite in the soil surrounding the Spektakel mine, Northern Cape Province, South Africa

[摘要] ENGLISH ABSTRACT: The Northern Cape Province of South Africa has played host to numerous mining activities for over a century. To date, most of the mining activity has ceased, leaving the area laden with derelict mine sites and unlined tailings dumps. One such site is the Spektakel mine situated to the west of the town of Springbok. The unlined copper and sulphide rich tailings at the site have the potential to leach elevated concentrations of copper and acidic water into the Buffels River downslope of the site. This poses a threat to the surrounding communities that rely mainly on the river to supply water for drinking, livestock and irrigation.The soil surrounding the tailings dumps was characterised in terms of its mineralogical and chemical properties. The results indicate that the soil contains elevated concentrations of Cu2+, which is bound in the soil in the form of the secondary copper hydroxy mineral atacamite (Cu2(OH)3Cl). No other secondary copper minerals were identified at the site. Analysis of the solution present on the surface of the tailings dumps indicate that the tailings are the main source of the high Cu2+, Mg2+ and SO42- concentrations observed in the surrounding soils. As this solution migrates through the tailings dumps, into the soil, it accumulates Cl- through halite dissolution. The resulting acidic Cu2+, Mg2+, SO42- and Cl- solution reacts with the calcite in the soil, replacing it with atacamite.To determine why only a copper chloride mineral formed in the sulphate rich environment a synthetic solution with the composition of a solution in equilibrium with the soil was evaporated, both in the presence and absence of calcite. The results indicate that when the solution comes into contact with calcite, atacamite immediately precipitated, removing the Cu2+ from the solution. In the absence of calcite Cu2+ remains conservative, accumulating in the solution without precipitating a copper sulphate mineral. This establishes that the elevated Mg2+ concentration of the solution induces the formation MgSO4 aqueous complexes that reduce the activity of free sulphate, thus restricting copper sulphate mineral formation.The results from the soil characterization indicate that the atacamite stabilization mechanisms (circumneutral pH, high Cl- concentration and calcite) in the soil are diminishing. During sporadic rain events the acidic tailings solutions dissolve the calcite and temporarily reduce the Cl- concentration of the soil. To determine how these decreases will influence Cu2+ mobility in the soil, the stability of atacamite was tested by reducing the pH both in the presence and the absence of chloride. The results indicate that an elevated Cl- concentration and a pH > 6 stabilizes atacamite. A decrease in either of these parameters destabilizes atacamite and favours its dissolution. The study concludes that the current chemical conditions in the soil at Spektakel favour the stability of atacamite. However, continued sporadic rain events will reduce the Cl- concentration in the soil by increasing the SO42- concentration. This acidic solution will dissolve the calcite in the soil, thus reducing the buffering capacity of the soil, leading to the instability of atacamite, resulting in the leaching of large quantities of Cu2+ into the surrounding water bodies.

[发布机构] Stellenbosch University