Abstract
Natural iron minerals and zero-valent metals have been widely tested as catalysts for the Fenton-like process, but the systematical comparison study about their catalytic performance was rarely conducted, and the risk of the secondary pollution of toxic heavy metals was still not uncertain. In this paper, a comparison study of applying pyrite, ilmenite, vanadium titano-magnetite (VTM), zero-valent iron (ZVI), and zero-valent copper (ZVC) as Fenton-like catalysts for the removal of imidacloprid was performed. The results showed that ZVI exhibited the highest activity among the recyclable solid catalysts with a removal rate of 96.8% at initial pH 3 using 10.78 mmol/L H2O2, due to iron corrosive dissolution. Vanadium titano-magnetite (VTM) exhibited the best activity at first use among tested minerals but with low reusability. Pyrite with stable morphology showed a medium but sustainable ability to degrade imidacloprid, achieving a removal rate of 10.5% in the fifth use. The reaction much favored the acidic condition of initial pH around 2 or 3. Meanwhile, there was a significant positive correlation between removal efficiency and dissolved Fe or Cu concentration. Pyrite was considered to be a promising catalyst in Fenton-like reaction. It was suggested that the system proceeded predominantly through a homogeneous route via dissolved Fe or Cu ions. Except ZVC and VTM, other tested catalysts showed the low possibility of causing secondary pollution of toxic metals in the application of Fenton-like process.
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Funding
The research was financially supported by the Natural Science Foundation of Jiangxi Province (20202BABL213024), the Scientific Research Fund of Jiangxi Provincial Education Department (GJJ190229), and the Doctoral Research Fund of the Jiangxi Agricultural University (Project No.9232307058).
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Siwan Liu, Wenwei Yu, and Huang Cai conducted the main experiments. Faying Lai and Huajun Huang interpreted the study of leached toxic heavy metals. Hansun Fang did the analysis of imidacloprid degradation mechanism. Jinbao He designed the whole experiment and wrote the manuscript. All authors read and approved the final manuscript.
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Chemical structure of imidacloprid; Photograph of natural minerals and zero-valent metals; Characteristics of simulated imidacloprid wastewater; UV-visible spectrum of the prepared wastewater; linear fitting result of the relationship between imidacloprid concentration and the absorbance at 270 nm; UV-visible spectra of the solutions after removing the metallic sludge in alkaline condition; SEM images of fresh and five-times-used ilmenite, VTM, ZVC as well as EDS image and elemental composition of them; textural properties of the studied materials; the concentrations of dissolved Cu and Fe after consecutive reactions at initial pH 3; total ion chromatogram from GC–MS analysis of the ZVI treated sample. (DOCX 10971 kb)
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Liu, S., Yu, W., Cai, H. et al. A comparison study of applying natural iron minerals and zero-valent metals as Fenton-like catalysts for the removal of imidacloprid. Environ Sci Pollut Res 28, 42217–42229 (2021). https://doi.org/10.1007/s11356-021-13731-x
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DOI: https://doi.org/10.1007/s11356-021-13731-x