Nitrate removal to its fate in wetland mesocosm filled with sponge iron: Impact of influent COD/N ratio

Highlights

• CW-Fe allowed a high-performance of NO₃^‒-N removal at the COD/N ratio of 0.

• Higher COD/N resulted in lower chem-denitrification and higher bio-denitrification.

• The application of s-Fe⁰ contributed to TIN removal in wetland mesocosm.

• s-Fe⁰ changed the main denitrifiers in wetland mesocosm.

Abstract

Sponge iron (s-Fe⁰) is a porous metal with the potential to be an electron donor for denitrification. This study aims to evaluate the feasibility of using s-Fe⁰ as the substrate of wetland mesocosms. Here, wetland mesocosms with the addition of s-Fe⁰ particles (CW-Fe) and a blank control group (CW-CK) were established. The NO₃^‒-N reduction property and water quality parameters (pH, DO, and ORP) were examined at three COD/N ratios (0, 5, and 10). Results showed that the NO₃^‒-N removal efficiencies were significantly increased by 6.6 to 58.9% in the presence of s-Fe⁰. NH₄⁺-N was mainly produced by chemical denitrification, and approximately 50% of the NO₃^‒-N was reduced to NH₄⁺-N, at the COD/ratio of 0. An increase of the influent COD/N ratio resulted in lower chemical denitrification and higher bio-denitrification. Although chemical denitrification mediated by s-Fe⁰ led to an accumulation of NH₄⁺-N at COD/N ratios of 0 and 5, the TIN removal efficiencies increased by 4.5%‒12.4%. Moreover, the effluent pH, DO, and ORP values showed a significant negative correlation with total Fe and Fe (II) (P<0.01). High-throughput sequencing analysis indicated that Trichococcus (77.2%) was the most abundant microorganism in the CW-Fe mesocosm, while Thauera, Zoogloea, and Herbaspirillum were the primary denitrifying bacteria. The denitrifiers, Simplicispira, Dechloromonas, and Denitratisoma, were the dominant bacteria for CW-CK. This study provides a valuable method and an improved understanding of NO₃^‒-N reduction characteristics of s-Fe⁰ in a wetland mesocosm.

Graphical abstract

Keywords

Sponge iron / Wetland mesocosm / Electronic donor / Denitrification / COD/N ratio

References

[1] Adav S S, Lee D J, Lai J Y (2010). Enhanced biological denitrification of high concentration of nitrite with supplementary carbon source. Applied Microbiology and Biotechnology, 85(3): 773–778

[2] An Y, Li T, Jin Z, Dong M, Li Q, Wang S (2009). Decreasing ammonium generation using hydrogenotrophic bacteria in the process of nitrate reduction by nanoscale zero-valent iron. Science of the Total Environment, 407(21): 5465–5470

[3] Claus G, Kutzner H J (1985). Denitrification of nitrate and nitric acid with methanol as carbon source. Applied Microbiology and Biotechnology, 22(5): 378–381

[4] Hao T, Li W, Lu H, Chui H, Mackey H R, van Loosdrecht M C, Chen G (2013). Characterization of sulfate-reducing granular sludge in the SANI(®) process. Water Research, 47(19): 7042–7052

[5] Her J J, Huang J S (1995). Influences of carbon source and C/N ratio on nitrate/nitrite denitrification and carbon breakthrough. Bioresource Technology, 54(1): 45–51

[6] Huang G, Liu F, Yang Y, Kong X, Li S, Zhang Y, Cao D (2015). Ammonium-nitrogen-contaminated groundwater remediation by a sequential three-zone permeable reactive barrier (multibarrier) with oxygen-releasing compound (ORC)/clinoptilolite/spongy iron: column studies. Environmental Science and Pollution Research International, 22(5): 3705–3714

[7] Ilyas H, Masih I (2017). The performance of the intensified constructed wetlands for organic matter and nitrogen removal: A review. Journal of Environmental Management, 198(Pt 1): 372–383

[8] Jiang C, Xu X, Megharaj M, Naidu R, Chen Z (2015). Inhibition or promotion of biodegradation of nitrate by Paracoccus sp. in the presence of nanoscale zero-valent iron. Science of the Total Environment, 530-531: 241–246

[9] Ju Y, Liu X, Liu R, Li G, Wang X, Yang Y, Wei D, Fang J, Dionysiou D D (2015). Environmental application of millimeter-scale sponge iron (s-Fe⁰) particles (II): The effect of surface copper. Journal of Hazardous Materials, 287: 325–334

[10] Khalil A M E, Eljamal O, Saha B B, Matsunaga N (2018). Performance of nanoscale zero-valent iron in nitrate reduction from water using a laboratory-scale continuous-flow system. Chemosphere, 197: 502–512

[11] Lee D W, Lee S D (2008). Tessaracoccus flavescens sp. nov., isolated from marine sediment. International Journal of Systematic and Evolutionary Microbiology, 58(4): 785–789

[12] Li B, Irvin S (2007). The comparison of alkalinity and ORP as indicators for nitrification and denitrification in a sequencing batch reactor (SBR). Biochemical Engineering Journal, 34(3): 248–255

[13] Li J, Li J, Li Y (2009). Cadmium removal from wastewater by sponge iron sphere prepared by charcoal direct reduction. Journal of Environmental Sciences (China), 21(Suppl 1): S60–S64

[14] Liu Y, Lowry G V (2006). Effect of particle age (Fe⁰ content) and solution pH on NZVI reactivity: H₂ evolution and TCE dechlorination. Environmental Science & Technology, 40(19): 6085–6090

[15] Mao Y, Xia Y, Wang Z, Zhang T (2014). Reconstructing a Thauera genome from a hydrogenotrophic-denitrifying consortium using metagenomic sequence data. Applied Microbiology and Biotechnology, 98(15): 6885–6895

[16] Mao Y, Xia Y, Zhang T (2013). Characterization of Thauera-dominated hydrogen-oxidizing autotrophic denitrifying microbial communities by using high-throughput sequencing. Bioresource Technology, 128(1): 703–710

[17] Mielcarek A, Rodziewicz J, Janczukowicz W, Dulski T, Ciesielski S, Thornton A (2016). Denitrification aided by waste beer in anaerobic sequencing batch biofilm reactor (AnSBBR). Ecological Engineering, 95: 384–389

[18] Negri E D, Alfano O M, Chiovetta M G (1995). Moving-Bed Reactor Model for the direct reduction of hematite. Parametric study. Industrial & Engineering Chemistry Research, 34(12): 4266–4276

[19] Nguyen N H A, Špánek R, Kasalický V, Ribas D, Vlková D, Řeháková H, Kejzlar P, Ševců A (2018). Different effects of nano-scale and micro-scale zero-valent iron particles on planktonic microorganisms from natural reservoir water. Environmental Science. Nano, 5(5): 1117–1129

[20] Panda L, Das B, Rao D S, Mishra B K (2011). Application of dolochar in the removal of cadmium and hexavalent chromium ions from aqueous solutions. Journal of Hazardous Materials, 192(2): 822–831

[21] Rahman M M, Roberts K L, Grace M R, Kessler A J, Cook P L M (2019). Role of organic carbon, nitrate and ferrous iron on the partitioning between denitrification and DNRA in constructed stormwater urban wetlands. Science of the Total Environment, 666: 608–617

[22] Shin K H, Cha D K (2008). Microbial reduction of nitrate in the presence of nanoscale zero-valent iron. Chemosphere, 72(2): 257–262

[23] Si Z, Song X, Wang Y, Cao X, Zhao Y, Wang B, Chen Y, Arefe A (2018). Intensified heterotrophic denitrification in constructed wetlands using four solid carbon sources: Denitrification efficiency and bacterial community structure. Bioresource Technology, 267: 416–425

[24] Tosco T, Petrangeli Papini M, Cruz Viggi C,Sethi R. (2014). Nanoscale zerovalent iron particles for groundwater remediation: A review. Journal of Cleaner Production, 77: 10–21

[25] Vymazal J (2007). Removal of nutrients in various types of constructed wetlands. Science of the Total Environment, 380(1-3): 48–65

[26] Wang G, Wang Y, Guo Y, Peng D (2017). Effects of four different phosphorus-locking materials on sediment and water quality in Xi’an moat. Environmental Science and Pollution Research International, 24(1): 264–274

[27] Wang G B, Wang Y, Zhang Y (2018). Combination effect of sponge iron and calcium nitrate on severely eutrophic urban landscape water: An integrated study from laboratory to fields. Environmental Science and Pollution Research International, 25(9): 8350–8363

[28] Yi Z, Xu J, Chen M, Li W, Yao J, Chen H, Wang F (2013). Removal of uranium(VI) from aqueous solution using sponge iron. Journal of Radioanalytical and Nuclear Chemistry, 298(2): 955–961

[29] Zhang Y, Douglas G B, Pu L, Zhao Q, Tang Y, Xu W, Luo B, Hong W, Cui L, Ye Z (2017). Zero-valent iron-facilitated reduction of nitrate: Chemical kinetics and reaction pathways. Science of the Total Environment, 598: 1140–1150

[30] Zhao Y, Cao X, Song X, Zhao Z, Wang Y, Si Z, Lin F, Chen Y, Zhang Y (2018). Montmorillonite supported nanoscale zero-valent iron immobilized in sodium alginate (SA/Mt-NZVI) enhanced the nitrogen removal in vertical flow constructed wetlands (VFCWs). Bioresource Technology, 267: 608–617

[31] Zhen Z, Qiao W, Xing C, Ying A, Shen X, Ren W, Jiang L M, Wang L (2015). Microbial community structure of anoxic–oxic-settling-anaerobic sludge reduction process revealed by 454-pyrosequencing. Chemical Engineering Journal, 266(12): 249–257

[32] Zhong Y, Yang Q, Fu G, Xu Y, Cheng Y, Chen C, Xiang R, Wen T, Li X, Zeng G (2018). Denitrifying microbial community with the ability to bromate reduction in a rotating biofilm-electrode reactor. Journal of Hazardous Materials, 342: 150–157

[33] Zhou J, Wang H, Yang K, Ji B, Chen D, Zhang H, Sun Y, Tian J (2016). Autotrophic denitrification by nitrate-dependent Fe(II) oxidation in a continuous up-flow biofilter. Bioprocess and Biosystems Engineering, 39(2): 277–284

Acknowledgements

This work was supported by the the National Natural Science Foundation of China (Grant Nos. 51679041 and 51909034); the Fundamental Research Funds for the Central Universities (Grant Nos. 2232019D3-21 and 2232018D3-22); the China Postdoctoral Science Foundation (No. 2018M641894); the Fundamental Research Funds for the Central Universities and Graduate Student Innovation Fund of Donghua University (Nos. CUSF-DH-D-2019079 and CUSF-DH-D-2019080); Shanghai Sailing Program (No. 19YF1401900); Shanghai Rising-Star Program (No. 19QC1401100).

RIGHTS & PERMISSIONS

2020 Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature