High temperature gas–solid reactions in calc–silicate Cu–Au skarn formation; Ertsberg, Papua Province, Indonesia

The 2.7–3 Ma Ertsberg East Skarn System (Indonesia), adjacent to the giant Grasberg Porphyry Copper deposit, is part of the world’s largest system of Cu–Au skarn deposits. Published fluid inclusion and stable isotope data show that it formed through the flux of magma-derived fluid through contact metamorphosed carbonate rock sequences at temperatures well above 600° C and pressures of less than 50 MPa. Under these conditions, the fluid has very low density and the properties of a gas. Combining a range of micro-analytical techniques, high-resolution QEMSCAN mineral mapping and computer-assisted X-ray micro-tomography, an array of coupled gas–solid reactions may be identified that controlled reactive mass transfer through the ~ 1 km³ hydrothermal skarn system. Vacancy-driven mineral chemisorption reactions are identified as a new type of reactive transport process for high-temperature skarn alteration. These gas–solid reactions are maintained by the interaction of unsatisfied bonds on mineral surfaces and dipolar gas-phase reactants such as SO₂ and HCl that are continuously supplied through open fractures and intergranular diffusion. Principal reactions are (a) incongruent dissolution of almandine-grossular to andradite and anorthite (an alteration mineral not previously recognized at Ertsberg), and (b) sulfation of anorthite to anhydrite. These sulfation reactions also generate reduced sulfur with consequent co-deposition of metal sulfides. Diopside undergoes similar reactions with deposition of Fe-enriched pyroxene in crypto-veins and vein selvedges. The loss of calcium from contact metamorphic garnet to form vein anhydrite necessarily results in Fe-enrichment of wallrock, and does not require Fe-addition from a vein fluid as is commonly assumed.