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Significance of Iron(II,III) Hydroxycarbonate Green Rust in Arsenic Remediation Using Zerovalent Iron in Laboratory Column Tests
Su, C. AND R W. Puls*. Significance of Iron(II,III) Hydroxycarbonate Green Rust in Arsenic Remediation Using Zerovalent Iron in Laboratory Column Tests. 10.1021/es0495462, J. Schnoor (ed.), ENVIRONMENTAL SCIENCE AND TECHNOLOGY. American Chemical Society, Washington, DC, 38(19):5224-5231, (2004).
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We examined the corrosion products of zerovalent iron used in three column tests for removing arsenic from water under dynamic flow conditions. Each column test lasted three- to four-months using columns consisting of a 10.3-cm depth of 50 : 50 (w : w, Peerless iron : sand) in the middle and a 10.3-cm depth of a sediment from Elizabeth City, NC in both upper and lower portions of the 31-cm long glass column (2.5 cm in diameter). The feeding solutions were 1 mg of As(V) L-1 + 1 mg of As(III) L-1 in 7 mM NaCl + 0.86 mM CaSO4 with or without added phosphate (0.5 or 1 mg of P L-1) and silicate (10 or 20 mg of Si L-1) at pH 6.5. Iron(II, III) hydroxycarbonate green rust (or simply, carbonate green rust) and magnetite were the major iron corrosion products identified with X-ray diffraction for the separated fractions (5 min and 1 min sedimentation, and residual). The presence of carbonate green rust was confirmed by scanning electron microscopy (hexagonal morphology) and FTIR-photo acoustic spectroscopy (interlayer carbonate stretching mode at 1352-1365 cm-1). X-ray photoelectron spectroscopy investigation revealed the presence of predominantly As(V) at the surface of corroded iron particles despite the fact that the feeding solution in contact with Peerless iron contained more As(III) than As(V) as a result of a preferential uptake of As(V) over As(III) by the Elizabeth City sediment. Extraction of separated corrosion products with 1.0 M HCl showed that from 86 to 96% of the total extractable As (6.9 to 14.6 g kg-1) was in the form of As(V) in agreement with the XPS results. Combined microscopic and macroscopic wet chemistry results suggest that sorbed As(III) was partly oxidized by the carbonate green rust. The column experiments suggest that either carbonate green rust is kinetically favored or is thermodynamically more stable than sulfate green rust in the studied Peerless iron corrosion systems.