Geochimica et Cosmochimica Acta
Geochimica et Cosmochimica Acta
5 years ago

Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions

Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions
Adsorption and redox reactions occur between arsenic-containing pyrite and arsenate, which affect the migration and conversion of arsenic in soils and waters. However, the influence of arsenic incorporated in pyrite on the interaction processes is still enigmatic. In this work, arsenic-containing pyrites were hydrothermally synthesized with composition similar to naturally surface-oxidized pyrites in supergene environments. The effects of arsenic incorporation on the chemical composition and physicochemical properties were analyzed, and the interaction mechanism between arsenic-containing pyrites and aqueous arsenate was also studied within pH 3.0–11.0. Arsenic-containing pyrites with the arsenic contents of 0 (Apy0), 4.4 (Apy5) and 9.9 wt.% (Apy10) were produced in hydrothermal systems. As(III) and As(−I) respectively substituted Fe(II) and S2(−II) in the pyrite, and their relative contents respectively reached 76.6% and 17.2% in Apy5, and 91.0% and 8.0% in Apy10. Arsenic substitution resulted in a high content of Fe(III) in the form of Fe(III)S and a decrease in pyrite crystallinity. During the redox processes of arsenic-containing pyrites and arsenate, elemental S0, SO4 2− and goethite were formed as the main products with the adsorption of As(III,V), and As(III) was released due to the collapse of the crystal structure of pyrite and the oxidation of As(−I). Different redox mechanisms were achieved with pH increasing from 3.0 to 11.0 in the reaction system. At pH 3.0–6.0, Fe(III) contributed much to the oxidation of arsenic-containing pyrites, and arsenate and released As(III) were adsorbed on the surface of solid products. At pH 7.0–11.0, aqueous arsenate worked as the major oxidant, and its oxidation capacity increased with increasing pH. When the pH was increased from 3.0 to 7.0 and 11.0, the release ratio of incorporated arsenic from Apy10 particles increased from 34.1% to 45.0% and 56.8%, respectively. The present study facilitates a better understanding about the interaction mechanisms between arsenic-containing pyrite and arsenate in supergene environments.

Publisher URL: www.sciencedirect.com/science

DOI: S0016703717305227

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