The migration and conversion of arsenic in the environment usually accompany by the redox of iron-bearing minerals. For instance, the oxidation of pyrite can generate reactive oxygen species (ROS) affecting the species of arsenic, but the types and roles of ROS have been unclear. This paper demonstrated the vital role of Fe(II) in the pyrite for the formation of ROS. Results showed that exogenous addition of Fe(II) significantly enhanced the removal rate of As(III) by pyrite. 2,2'-bipyridine (BPY) decreased the oxidation of As(III) by complexing with Fe2+ in solution, whilst EDTA enhanced the oxidation of As(III) by boosting the autoxidation of Fe2+. In addition, neutral pH is superior for the oxidation of As(III) and removal of total arsenic. Importantly, Methanol, SOD enzyme and PMOS inhibited 54%, 28% and 17.5% of As(III) oxidation, respectively, which indicated O2•- and •OH were the main contributors to As(III) oxidation, and Fe(IV) contributed a small part of As(III) oxidation. The content of As(V) in the FeS2-Fe2+-As(III) system was higher than that in the FeS2-As(III) system, further confirming the vital role of Fe(II) for As(III) oxidation. Lepidocrocite was produced in a single Fe2+ system, which was not detected in the FeS2-As(III) system. Thus, the presence of mineral surfaces changed the oxidation products of Fe2+ and accelerated the oxidation and immobilization of As(III). FA (Fulvic Acid) and HA (Humic Acid) accelerated the oxidation of As(III), but the oxidation of As(III) by pyrite was inhibited to a certain extent, with increasing phenolic hydroxyl groups in phenolic acid. Our findings provide new insight into the oxidative species in the pyrite-Fe(II) system and will help guide the remediation of arsenic pollution in complex environmental systems.
Keywords: Arsenic redox transformation; Co-oxidation; Free radicals; Kinetics.
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