Os isotopic composition and Os and Re distribution in the active mound of the TAG hydrothermal system, Mid-Atlantic Ridge

Drilling during ODP Leg 158 took place on the active mound of the TAG hydrothermal field on the Mid-Atlantic Ridge. The dominant mineral precipitating from the hydrothermal fluid is pyrite. Its Re and Os concentration and the Os isotopic composition provide constraints on the nature of the hydrothermal fluid circulating in the TAG mound. The 187Os/186Os ratios of massive pyrite samples vary from 4.9 to 8.9. The highest ratios have been observed in the upper part of the sulfide mountain (<20 mbsf) and the lowest in the stockwork zone at ~80 mbsf. This range of Os isotopic compositions is likely the result of mixing of seawater with hydrothermal fluid. The Os concentrations are very low, ranging from 0.04 to 4.2 ppt, and the massive pyrite zone at the top of the mound is enriched in Os relative to the interior of the hydrothermal system. A hyperbolic relationship between Os isotopic composition and Os concentration reflects the systematic addition of seawater-derived Os to the hydrothermal Os component at stratigraphically shallower levels. From this relationship it is estimated that pyrite precipitating from the hydrothermal fluid contains 0.02 to 0.04 ppt Os provided the 187Os/186Os value of the fluid ranges from about 1.3 to 4.7. Because of the great mobility of Os in the high-temperature hydrothermal system, it is assumed that its partition coefficient between pyrite and hydrothermal fluid is <1. This implies that the hydrothermal fluid contains more than 0.02 ppt Os. The occurrence of anhydrite-rich lithologies at ~30–40 mbsf corroborates that seawater is penetrating the hydrothermal system and contaminating the hydrothermal fluid circulating in the upper part of the mound. This partly explains why the Os of sulfides that precipitated above this level has a strong seawater-like isotopic signature. In addition, the massive pyrite zone of the upper part of the TAG mound formed by accumulation of sulfides derived from chimneys and the fall-out material of the hydrothermal plume above the TAG field. Both sulfide components formed during mixing of seawater and hydrothermal fluid and their Os should also have a distinct seawater component. These processes, especially the entrainment of seawater, appear to control the distribution of Os and Re within the hydrothermal system. The Os enrichment in the upper part of the mound can be explained if the element is co-precipitated with sulfides or adsorbed on mineral surface during the accumulation of sulfides on the TAG mound. As a significant amount of Os can be dissolved in the hydrothermal fluid, remobilization of Os within the hydrothermal system could lead to further Os enrichment at the top of the mound but to very low Os concentrations in the stockwork zone. The Re concentrations indicate a distribution opposite to that of Os: the highest concentrations of about 60 ppb have been observed more than 15 mbsf, but the concentrations decrease from 50 to 2 ppb in samples from the top of the sulfide mound (