Pivotal effects of external Fe2+ on remediation of arsenite by zero-valent iron/persulfate: Efficiencies and mechanism

Persulfate could be activated by zero-valent iron (ZVI) leading to the rapid removal of various contaminants. However, quick consumption of Fe2+ largely constrained the removal (%) of target pollutants. Here it was reported that Na2S2O8 (SP) combined with ZVI, as an external source of Fe2+, was activated by Fe2+ to quickly (minutes scale) and efficiently (more than 90%) remove As (III) from aqueous solution at an initial pH value from 1.0 to 9.0. As (III) removal was obviously improved by an increase of Fe2+ rather than Na2S2O8 dosage. The removal of As (III) using Fe2+-SP-ZVI system followed the pseudo-second-order kinetic and pseudo-first-order kinetic expression. Fe2+ from ZVI oxidization could improve the efficient generation of SO4 center dot-, which obviously boosted ZVI corrosion. The production of SO4 center dot- could be manipulated by oxalic acid, ethylenediaminetetraacetic acid (EDTA), citric acid and phosphates through controlling the concentration of dissociative Fe2+, leading to an obvious repression on As (III) removal. The fitting of X-ray absorption fine structure (XAFS) spectra illustrated that the interatomic distance of As-O shell was located between As(III)-O and As(V)-O shell and external Fe2+ could promote the oxidation of As (III) to As (V) from 35.6% in 1.0 min-44.5% in 10.0 min. Goethite as the main component of iron oxyhydroxides might play a significant role of As (III) adsorption in Fe2+-SP-ZVI system. These findings are crucial for knowing the fate and transport of arsenic under permeable reactive barriers.