Evolution of nanoscale zero-valent iron (nZVI) in water: Microscopic and spectroscopic evidence on the formation of nano- and micro-structured iron oxides

[Display omitted] •A comprehensive study of corrosion products for nZVI under both oxic and anoxic conditions is performed.•Under anoxic conditions, the oxidation products contain a mixture of wustite (FeO), goethite (α-FeOOH) and akaganeite (β-FeOOH).•Under oxic conditions, the final products are mainly crystalline lepidocrocite (γ-FeOOH) with acicular-shaped structures.•Morphological and structural evolution of nZVI under both oxic and anoxic conditions are substantially different. Knowledge on the transformation of nanoscale zero-valent iron (nZVI) in water is essential to predict its surface chemistry including surface charge, colloidal stability and aggregation, reduction and sorption of organic contaminants, heavy metal ions and other pollutants in the environment. In this work, transmission electronic microscopy (TEM), X-ray diffraction (XRD) and Raman spectroscopy are applied to study the compositional and structural evolution of nZVI under oxic and anoxic conditions. Under anoxic conditions, the core–shell structure of nZVI is well maintained even after 72h, and the corrosion products usually contain a mixture of wustite (FeO), goethite (α-FeOOH) and akaganeite (β-FeOOH). Under oxic conditions, the core–shell structure quickly collapses to flakes or acicular-shaped structures with crystalline lepidocrocite (γ-FeOOH) as the primary end product. This work provides detailed information and fills an important knowledge gap on the physicochemical characteristics and structural evolution of engineered nanomaterials in the environment.