Reactivity characterization of SiO2-coated nano zero-valent iron for iodoacetamide degradation: The effects of SiO2 thickness, and the roles of dehalogenation, hydrolysis and adsorption.
2022
Abstract The effect of SiO2-layer thickness in SiO2-coated nano zero-valent iron (nZVI) particles on the reactivity characteristics of iodoacetamide (IAcAm) degradation was evaluated. SiO2-layer thicknesses ranging from 3.6 to 27.3 nm were obtained through varying tetraethyl orthosilicate dosages of 0.001–1 M. The crystallinity, surface chemical composition, and physicochemical properties were evaluated for their effects on synergetic degradation mechanisms, dehalogenation, hydrolysis, and adsorption. At a thickness of 3.6 nm, the SiO2 layer offered the highest observed pseudo-first-order rate ( k o b s ) and higher rates of IAcAm degradation were maintained under pH fluctuations (pH 5–7) and aerobic conditions compared to pristine nZVI. At this SiO2-layer thickness (3.6 nm), the rate of iron oxide-layer formation was reduced and the migration of reactive iron species (Fe0 and Fe2+) for the dehalogenation and hydrolysis reactions was enabled. In a single-solute solution, IAcAm elimination was greater than bromoacetamide and chloroacetamide elimination due to the weak ionic I–C bond. In mixed solute conditions, the hydrophobicity of chloroacetamide played a more significant role in competitive degradation through greater adsorption. The proportion of dehalogenation relative to hydrolysis during IAcAm degradation by pristine nZVI and SiO2-coated nZVI was approximately 0.6:0.4. Iodoacetic acid and acetic acid were detected as intermediates in the degradation pathway of IAcAm by pristine nZVI. In contrast, the SiO2 layer on nZVI can accelerate the transformation of IAcAm to acetamide and iodoacetic acid. The electrolyte background of tap water exhibited a slight inhibitory effect on the degradation of IAcAm for both nZVI and SiO2-coated nZVI.
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