The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The fate of nitrogen and iron species

doi:10.1007/s11783-020-1366-2

Front. Environ. Sci. Eng.

2021, Vol. 15

Issue (4) : 73 https://doi.org/10.1007/s11783-020-1366-2

RESEARCH ARTICLE

The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The fate of nitrogen and iron species

Boyi Cheng¹, Yi Wang¹, Yumei Hua¹(

), Kate V. Heal²

¹. College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China
². School of GeoSciences, University of Edinburgh, Edinburgh EH9 3FF, UK

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Abstract

•Bacterially-mediated coupled N and Fe processes examined in incubation experiments.

•NO₃⁻ reduction was considerably inhibited as initial Fe/N ratio increased.

•The maximum production of N₂ occurred at an initial Fe/N molar ratio of 6.

•Fe minerals produced at Fe/N ratios of 1–2 were mainly easily reducible oxides.

The Fe/N ratio is an important control on nitrate-reducing Fe(II) oxidation processes that occur both in the aquatic environment and in wastewater treatment systems. The response of nitrate reduction, Fe oxidation, and mineral production to different initial Fe/N molar ratios in the presence of Paracoccus denitrificans was investigated in 132 h incubation experiments. A decrease in the nitrate reduction rate at 12 h occurred as the Fe/N ratio increased. Accumulated nitrite concentration at Fe/N ratios of 2–10 peaked at 12–84 h, and then decreased continuously to less than 0.1 mmol/L at the end of incubation. N₂O emission was promoted by high Fe/N ratios. Maximum production of N₂ occurred at a Fe/N ratio of 6, in parallel with the highest mole proportion of N₂ resulting from the reduction of nitrate (81.2%). XRD analysis and sequential extraction demonstrated that the main Fe minerals obtained from Fe(II) oxidation were easily reducible oxides such as ferrihydrite (at Fe/N ratios of 1–2), and easily reducible oxides and reducible oxides (at Fe/N ratios of 3–10). The results suggest that Fe/N ratio potentially plays a critical role in regulating N₂, N₂O emissions and Fe mineral formation in nitrate-reducing Fe(II) oxidation processes.

Keywords Denitrification N₂O emission Fe(II) oxidation Fe/N ratio Fe minerals

Corresponding Author(s): Yumei Hua

Issue Date: 12 November 2020

Cite this article:

Boyi Cheng,Yi Wang,Yumei Hua, et al. The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The fate of nitrogen and iron species[J]. Front. Environ. Sci. Eng., 2021, 15(4): 73.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1366-2
https://academic.hep.com.cn/fese/EN/Y2021/V15/I4/73

Fig.1 Schematic representation of the sampling and pretreatment processes for gas, liquids, and precipitates from the experimental bottles.

Fig.2 NO₃⁻ concentration (a), NO₂⁻ concentration (b), and NO₂⁻ accumulation expressed as a % of NO₃⁻ reduction (c) during the incubation. The NO₂⁻ concentration at a Fe/N ratio of 1 was zero throughout the incubation, and that at a Fe/N ratio of 2 fell to zero after 36 h. Values are means (n = 3) and error bars in (a) and (b) represent the standard deviation.

Fig.3 N₂O production (a) and N₂ production (b) in the headspace at different Fe/N ratios during the incubation.

Fig.4 Dissolved Fe(II) concentrations (a), dissolved Fe(III) concentrations (b) during the incubation, and consumption percentages of Fe(II) at 132 h (c). Values are means (n = 3) and error bars in (a), (b) and (c) represent the standard deviation.

Fig.5 FESEM images of precipitates from treatments with different Fe/N ratios at 60 h. (a) Fe/N=1:1, (b) Fe/N=2:1, (c) Fe/N=3:1, (d) Fe/N=4:1, (e) Fe/N=5:1, (f) Fe/N=6:1, (g) Fe/N=8:1 and (h) Fe/N=10:1. Green arrows indicate precipitates, and red arrows indicate small holes on cell surfaces.

Fig.6 X-ray diffraction patterns of the precipitates from different Fe/N ratio treatments at 12, 60 and 132 h. (a) Fe/N=1:1, (b) Fe/N=2:1, (c) Fe/N=3:1, (d) Fe/N=4:1, (e) Fe/N=5:1, (f) Fe/N=6:1, (g) Fe/N=8:1 and (h) Fe/N=10:1. V represents vivianite, G represents goethite, F represents ferrihydrite and M represents magnetite.

Fig.7 Fe speciation of the precipitates from different Fe/N ratio treatments after 132 h incubation. For explanation of the different Fe fractions in the legend see text in Section 2.3.

Fig.8 Possible mechanisms for the role of Fe minerals in the NRFO process mediated by bacteria. Chemodenitrification is indicated by red arrows and biological reduction is indicated by black arrows. Nar, nitrate reductase; Nir, nitrite reductase; Nor, nitric oxide reductase; Nos, nitrous oxide reductase.

Fig.9 Percentage contribution of the N products of denitrification (NO₂⁻, N₂O and N₂) to NO₃⁻ reduction from different Fe/N ratio treatments after 132 h incubation.

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