Hematite-facilitated microbial ammoxidation for enhanced nitrogen removal in constructed wetlands

doi:10.1007/s11783-024-1842-1

Front. Environ. Sci. Eng.

2024, Vol. 18

Issue (7) : 82 https://doi.org/10.1007/s11783-024-1842-1

Hematite-facilitated microbial ammoxidation for enhanced nitrogen removal in constructed wetlands

Hao Qin^1,², Wenbo Nie^1,², Duo Yi^1,², Dongxu Yang^1,², Mengli Chen³, Tao Liu^1,², Yi Chen^1,²(

)

¹. Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment (Ministry of Education), Chongqing University, Chongqing 400045, China
². College of Environment and Ecology, Chongqing University, Chongqing 400045, China
³. Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University, Chengdu 610031, China

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Abstract

● H-CWs synergistically eliminate NH₄⁺ and NO₃⁻ while reducing N₂O emissions.

● Inhibitors and isotope incubations are used to prove the Feammox process.

● Feammox contributes approximately 40% to ammonia removal in H-CWs.

● Nanowires on the hematite suggest ammoxidation likely linked to EET.

● H-CWs enhance the abundance of nitrogen-metabolizing microorganisms and genes.

Constructed wetlands (CWs) are widely applied for decentralized wastewater treatment. However, achieving efficient removal of ammonia (NH₄⁺–N) has proven challenging due to insufficient oxygen. In this study, natural hematite (Fe₂O₃) was employed as a CW substrate (H-CWs) for the first time to drive anaerobic ammonia oxidation coupled with iron(III) reduction (Feammox). Compared to gravel constructed wetlands (G-CWs), ammonia removal was enhanced by 38.14% to 54.03% and nitrous oxide (N₂O) emissions were reduced by 34.60% in H-CWs. The synergistic removal of ammonia and nitrate by H-CWs also resulted in the absence of ammoxidation by-products. Inhibitor and ¹⁵N isotope tracer incubations showed that Feammox accounting for approximately 40% of all ammonia removal in the H-CWs. The enrichment of iron phosphate (Fe₃Fe₄(PO₄)₆) promoted the accumulation of the Feammox intermediate compound FeOOH. Microbial nanowires were observed on the surface of H-CW substrates as well, suggesting that the observed biological ammoxidation was most likely related to extracellular electron transfer (EET). Microbial and metagenomics analysis revealed that H-CWs elevated the integrity and enhanced the abundance of functional microorganisms and genes associated with nitrogen metabolism. Overall, the efficient ammonia removal in the absence of O₂ together with a reduction in N₂O emissions as described in this study may provide useful guidance for hematite-mediated anaerobic ammonia removal in CWs.

Keywords Constructed wetlands Nitrogen removal Feammox Hematite Iron cycle

Corresponding Author(s): Yi Chen

About author:

Issue Date: 27 March 2024

Cite this article:

Hao Qin,Wenbo Nie,Duo Yi, et al. Hematite-facilitated microbial ammoxidation for enhanced nitrogen removal in constructed wetlands[J]. Front. Environ. Sci. Eng., 2024, 18(7): 82.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1842-1
https://academic.hep.com.cn/fese/EN/Y2024/V18/I7/82

Fig.1 Concentrations of ammonia nitrogen (NH₄⁺–N) in the influent and effluent of the CWs over the experimental period. Data are presented as mean ± standard deviation, n = 3. (H-CWs: hematite constructed wetlands; G-CWs: gravel constructed wetlands).

Fig.2 Nitrogen compound concentrations over time in batch experiments with initial influent nitrogen concentrations of 35 mg/L NH₄⁺–N (a) or 21 mg/L NO₃^?–N (b) with 21 mg/L NO₃^?–N or 35 mg/L NH₄⁺–N introduced after 24 h, respectively.

Fig.3 N₂O emission fluxes (n = 3) from CWs over 72 h when HRT = 3 d.

Fig.4 Mean ³⁰N₂ (a) and ²⁹N₂ (b) production rates of CWs substrates under inhibitor and 10% ¹⁵N isotope incubation (n = 3). (ATU: allylthiourea, a nitrification process inhibitor; BDI: procyanidins, a biological denitrification inhibitor).

Fig.5 XRD patterns of the initial hematite and hematite substrate (a) and high-resolution spectra for the XPS peaks of Fe2p (b). * and ● indicate FeOOH and Fe₃Fe₄(PO₄)₆, respectively.

Fig.6 SEM images of gravel substrate (a), initial hematite (b), and hematite substrate (c, d). (Magnification resp. A/D: 10 k, B/C: 20 k).

Fig.7 Relative abundances of the top 10 microorganisms in CWs at the phylum (a) and genus (b) levels. Pearson correlation coefficients between nitrogen compounds, Fe(III), and microorganisms (c).

Fig.8 Relative abundance (‰) of functional genes associated with nitrogen compounds transformation (a). Nitrogen compound transformation relationships of the H-CWs based on relative abundance (b). The varying thickness of the lines depicts the abundance of genes, with dashed lines denoting the absence or unconfirmed status of the metabolic pathway and the question marks denoting genes that are yet to be identified or confirmed.

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