Mechanistic study for stibnite oxidative dissolution and sequestration on pyrite
2020
Yan, Li | Chan, Tingshan | Jing, Chuanyong
Stibnite (Sb₂S₃) dissolution and transformation on mineral surfaces are the fundamental steps controlling the fate of antimony (Sb) in the environment. The molecular-level understanding of Sb₂S₃-mineral-water interfacial reactions is of great importance. Herein, Sb₂S₃ oxidative dissolution and sequestration on pyrite (FeS₂) were explored. The results show that FeS₂ accelerated the rate of Sb₂S₃ oxidative dissolution by a factor of 11.4-fold under sunlight due to heterogeneous electron transfer. The electron transfer from Sb₂S₃ to FeS₂ separated photogenerated hole (h⁺) and electron (e⁻) pairs, facilitating the generation of hydroxyl radicals (OH) on Sb₂S₃ and FeS₂, and superoxide radicals (O₂⁻) on FeS₂. Surface O₂⁻ was the dominant oxidant for Sb(III) oxidation with 91% contribution, as evidenced by radical trapping experiments. OH was preferentially adsorbed on Sb₂S₃, but was released with Sb₂S₃ dissolution, and subsequently contributable to Sb(III) oxidation in solution. The Sb(III) oxidation and sequestration on FeS₂ surface coupled Fe²⁺/Fe³⁺ cycling and inhibited FeS₂ dissolution, as evidenced by X-ray absorption near edge structure and X-ray photoelectron spectroscopy. The insights gained from this study further our understanding of Sb₂S₃ transformation and transport at the environmental mineral-water interfaces.
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