The solubility and speciation of gold in ammonia-bearing aqueous solutions at elevated temperature: An experimental study

Abstract

The discovery, using short wavelength infrared radiation (SWIR), that some low-sulfidation epithermal gold deposits are associated with hydrothermal alteration involving ammonium minerals, particularly buddingtonite ((NH4)AlSi3O8), has led to the suggestion that the gold may have been transported as a complex involving ammonia (NH3). The speciation of gold in ammonia-rich solutions, however, has received little attention from experimentalists and, consequently, it is not known whether gold forms stable complexes with NH3 and whether such species could contribute significantly to the transport of gold in epithermal ore-forming systems. To resolve this issue, we have conducted experiments to investigate the speciation and solubility of gold in ammonia-bearing solutions at temperatures of 225 and 250 °C under vapour-saturated water pressure with oxygen fugacity buffered by the assemblage magnetite-hematite. Based on the results of these experiments, gold does form stable species with ammonia at elevated temperature. The gold is interpreted to have been dissolved predominantly as Au(NH3)OH0 in solutions with a NH30 concentration of 0.005 ∼ 0.49 m and a pH(T) of 3.29 ∼ 7.47. This species formed via the reaction, Au (s) + NH3 (aq) + H2O = Au(NH3)OH(aq) + 1/2 H2 (g) The logarithms of the equilibrium constant for this reaction are −8.95 ± 0.84 and −7.71 ± 0.85 for 225 and 250 °C, respectively. In order to determine whether this species is important for the transport of gold in epithermal systems, we modeled the speciation of gold in a fluid at conditions typical of those epithermal gold depositing fluids. This modeling shows that the solubility of gold as AuHS0 and Au(HS)2- is much higher than that as Au(NH3)OH0 except in alkaline ammonia-bearing fluids. The association of gold mineralization with hydrothermal alteration involving the formation of ammonium-bearing minerals in the deposits is therefore probably unrelated to the transport of gold as a Au-NH3 complex but simply reflects the high concentration of NH4+ in the ore-forming fluid.