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Abstract

Pyrite is a ubiquitous sulfide mineral found in diverse geological settings and holds great significance in the formation of Au deposits as well as the safe utilization of groundwater due to its remarkable ability to incorporate substantial amounts of As. However, despite its importance, there remains a dearth of fundamental data on the partitioning of As between pyrite and fluid, which is key for accurately modeling the As distribution in these environments. Here, we present new insights into the partitioning behavior of As between pyrite and fluid at conditions that mimic natural fluid systems. Pyrite was synthesized by replacement of natural siderite in hydrothermal experiments at 200 °C and pH 5 applying a wide range of fluid As concentrations, spanning from 0.001 to 100 µg/g. The As distribution and concentration in synthetic pyrite was analyzed by quantitative LA-ICP-MS mapping providing a high spatial resolution and sensitivity at 2–3 µm image pixel size at a detection limit of ∼1 µg/g at the single pixel scale. Pyrite-fluid partitioning coefficients (DAs(py/fluid)) between synthetic pyrite and experimental fluid agree with previously published data for high fluid As concentrations of 1 µg/g to 100 µg/g (DAs < 2000). However, at low As concentrations in the experimental fluid (<1 µg/g), a steep increase in the DAs(py/fluid) values of up to ∼30,000 was detected, demonstrating even stronger As partitioning into pyrite. This is confirmed by the analyses of natural pyrite that precipitated from As-poor fluids (0.3–0.4 ng/g) within a deep anoxic aquifer in SE Sweden. The discovery holds significant implications for the mobility and scavenging of As, which in turn is important for understanding the formation and fingerprinting of mineral deposits as well as for the secure utilization of groundwater resources.