Abstract
Heterotrophic/autotrophic denitrification (HAD) is an effective approach to remove nitrate from contaminated groundwater. To improve its performance, easily degradable organics (methanol, ethanol, oxalic acid, and sodium acetate) and nano-zero valent iron (nZVI) were selected as co-electron donors for HAD, and their effectiveness in enhancing HAD to remove nitrate from simulated groundwater was evaluated. It was found that the removal efficiency of HAD to nitrate was significantly affected by the species of easily degradable organics as their different biological availability. Among the tested organics, ethanol-supported HAD system exhibited a better removal efficiency, and after 10 days reaction, it could achieve a high nitrate removal rate to 85.6% with an initial concentration of 90.94 mg/l, and at the end of the test (27 days), nitrate was almost completely removed in the interaction of heterotrophic denitrification (HD) and autotrophic denitrification (AD), and there was no nitrite and ammonium accumulation (< 0.1 and 1.0 mg/l). Moreover, the initial C/N ratios (0.2, 0.5, 1.0, 2.0, and 4.0) of simulated groundwater had a significant influence on nitrate removal by HAD. Increasing the C/N from 0.2 to 2.0 could markedly enhance nitrate removal efficiency, but continuously increased to 4.0 the removal rate just decreased; nevertheless, the accumulation of nitrite and ammonium were closely related to both the C/N ratios and species of organics. The synergistic effect between HD and AD process plays a vital role in the mixotrophic environment. Therefore, this research provides an effective method for nitrate removal from contaminated water with low organic carbon.
Similar content being viewed by others
References
Aminzadeh, B., Torabian, A., Azimi, A. A., Nabi Bidhendi, G. R. N., & Mehrdadi, N. (2010). Salt inhibition effects on simultaneous heterotrophic/autotrophic denitrification of high nitrate wastewater. International Journal of Environmental Research, 4, 255–262.
Camargo, J. A., & Alonso, Á. (2006). Ecological and toxicological effects of inorganic nitrogen pollution in aquatic ecosystems: a global assessment. Environment International, 32, 831–849.
Chen, J., Tang, C., Sakura, Y., Yu, J., & Fukushima, Y. (2005). Nitrate pollution from agriculture in different hydrogeological zones of the regional groundwater flow system in the North China plain. Hydrogeology Journal, 13, 481–492.
Della Rocca, C., Belgiorno, V., & Meriç, S. (2006). An heterotrophic/autotrophic denitrification (HAD) approach for nitrate removal from drinking water. Process Biochemistry, 41, 1022–1028.
Della Rocca, C., Belgiorno, V., & Meriç, S. (2007a). Overview of in-situ applicable nitrate removal processes. Desalination, 204, 46–62.
Della Rocca, C., Belgiorno, V., & Meriç, S. (2007b). Heterotrophic/autotrophic denitrification (HAD) of drinking water: prospective use for permeable reactive barrier. Desalination, 210, 194–204.
Ezzatahmadi, N., Ayoko, G. A., Millar, G. J., Speight, R., Yan, C., Li, J., Li, S., Zhu, J., & Xi, Y. (2017). Clay-supported nanoscale zero-valent iron composite materials for the remediation of contaminated aqueous solutions: a review. Chemical Engineering Journal, 312, 336–350.
Fang, Z., Qiu, X., Chen, J., & Qiu, X. (2011). Degradation of the polybrominated diphenyl ethers by nanoscale zero-valent metallic particles prepared from steel pickling waste liquor. Desalination, 267, 34–41.
Firth, S., Hildenbrand, B., & Morgan, P. (2014). Ethanol effects on the fate and transport of gasoline constituents in the UK. Science of the Total Environment, 485, 705–710.
Gómez, M. A., González-López, J., & Hontoria-Garcı́a, E. (2000). Influence of carbon source on nitrate removal of contaminated groundwater in a denitrifying submerged filter. Journal of Hazardous Materials, 80, 69–80.
Gao, L., Zhou, W., Huang, J., He, S., Yan, Y., Zhu, W., Wu, S., & Zhang, X. (2017). Nitrogen removal by the enhanced floating treatment wetlands from the secondary effluent. Bioresource Technology, 234, 243–252.
Ghafari, S., Hasan, M., & Aroua, M. K. (2008). Bio-electrochemical removal of nitrate from water and wastewater—a review. Bioresource Technology, 99, 3965–3974.
Gibert, O., Pomierny, S., Rowe, I., & Kalin, R. M. (2008). Selection of organic substrates as potential reactive materials for use in a denitrification permeable reactive barrier (PRB). Bioresource Technology, 99, 7587–7596.
Giordano, M. (2010). Global groundwater? Issues and solutions. Annual Review of Environment & Resources, 34, 153–178.
Gleeson, T., Wada, Y., Bierkens, M. F. P., & van Beek, L. P. H. (2012). Water balance of global aquifers revealed by groundwater footprint. Nature, 488, 197–200.
Harrison, I., Williams, G. M., & Carlick, C. A. (2003). Enantioselective biodegradation of mecoprop in aerobic and anaerobic microcosms. Chemosphere, 53, 539–549.
Hosseini, S. M., & Tosco, T. (2015). Integrating NZVI and carbon substrates in a non-pumping reactive wells array for the remediation of a nitrate contaminated aquifer. Journal of Contaminant Hydrology, 179, 182–195.
Hu, S., Wu, Y., Wang, L., Yao, H., & Li, T. (2014). Simultaneous removal of nitrate and aniline from groundwater by cooperating heterotrophic denitrification with anaerobic ammonium oxidation. Desalination & Water Treatment, 52, 7937–7950.
Hu, S., Yao, H., Wang, K., Lu, C., & Wu, Y. (2015). Intensify removal of nitrobenzene from aqueous solution using nano-zero valent iron/granular activated carbon composite as Fenton-like catalyst. Water Air & Soil Pollution, 226, 1–13.
Hu, S., Zhang, C., Yao, H., Lu, C., & Wu, Y. (2016). Intensify chemical reduction to remove nitrate from groundwater via internal microelectrolysis existing in nano-zero valent iron/granular activated carbon composite. Desalination & Water Treatment, 57, 14158–14168.
Huang, G., Fallowfield, H., Guan, H., & Liu, F. (2012). Remediation of nitrate-nitrogen contaminated groundwater by a heterotrophic-autotrophic denitrification approach in an aerobic environment. Water, Air, & Soil Pollution, 223, 4029–4038.
Hwang, Y.-H., Kim, D.-G., & Shin, H.-S. (2011). Mechanism study of nitrate reduction by nano zero valent iron. Journal of Hazardous Materials, 185, 1513–1521.
Khalil, A. M. E., Eljamal, O., Jribi, S., & Matsunaga, N. (2016). Promoting nitrate reduction kinetics by nanoscale zero valent iron in water via copper salt addition. Chemical Engineering Journal, 287, 367–380.
Khondaker, A. N., Al-Layla, R. I., & Husain, T. (1990). Groundwater contamination studies-the state-of-the-art. Critical Reviews in Environmental Control, 20, 231–256.
Kim, S. A., Kamala-Kannan, S., Lee, K.-J., Park, Y.-J., Shea, P. J., Lee, W.-H., Kim, H.-M., & Oh, B.-T. (2013). Removal of Pb(II) from aqueous solution by a zeolite–nanoscale zero-valent iron composite. Chemical Engineering Journal, 217, 54–60.
Liu, T., Yang, X., Wang, Z.-L., & Yan, X. (2013). Enhanced chitosan beads-supported Fe0-nanoparticles for removal of heavy metals from electroplating wastewater in permeable reactive barriers. Water Research, 47, 6691–6700.
Martínez, J., Ortiz, A., & Ortiz, I. (2017). State-of-the-art and perspectives of the catalytic and electrocatalytic reduction of aqueous nitrates. Applied Catalysis B: Environmental, 207, 42–59.
Menció, A., Mas-Pla, J., Otero, N., Regàs, O., Boy-Roura, M., Puig, R., Bach, J., Domènech, C., Zamorano, M., Brusi, D., & Folch, A. (2016). Nitrate pollution of groundwater; all right…, but nothing else? Science of the Total Environment, 539, 241–251.
Moussavi, G., Jafari, S. J., & Yaghmaeian, K. (2015). Enhanced biological denitrification in the cyclic rotating bed reactor with catechol as carbon source. Bioresource Technology, 189, 266–272.
Park, J.-H., Kim, S.-H., Delaune, R. D., Cho, J.-S., Heo, J.-S., Ok, Y. S., & Seo, D.-C. (2015). Enhancement of nitrate removal in constructed wetlands utilizing a combined autotrophic and heterotrophic denitrification technology for treating hydroponic wastewater containing high nitrate and low organic carbon concentrations. Agricultural Water Management, 162, 1–14.
Pfenning, K. S., & McMahon, P. B. (1997). Effect of nitrate, organic carbon, and temperature on potential denitrification rates in nitrate-rich riverbed sediments. Journal of Hydrology, 187, 283–295.
Ponder, S. M., Darab, J. G., Bucher, J., Caulder, D., Craig, I., Davis, L., Edelstein, N., Lukens, W., Nitsche, H., Rao, L., Shuh, D. K., & Mallouk, T. E. (2001). Surface chemistry and electrochemistry of supported zerovalent iron nanoparticles in the remediation of aqueous metal contaminants. Chemistry of Materials, 13, 479–486.
Repert, D. A., Barber, L. B., Hess, K. M., Keefe, S. H., Kent, D. B., LeBlanc, D. R., & Smith, R. L. (2006). Long-term natural attenuation of carbon and nitrogen within a groundwater plume after removal of the treated wastewater source. Environmental Science & Technology, 40, 1154–1162.
Rodríguez-Maroto, J. M., García-Herruzo, F., García-Rubio, A., Gómez-Lahoz, C., & Vereda-Alonso, C. (2009). Kinetics of the chemical reduction of nitrate by zero-valent iron. Chemosphere, 74, 804–809.
Simon, F. G., & Meggyes, T. (2000). Removal of organic and inorganic pollutants from groundwater using permeable reactive barriers: part 1. Treatment processes for pollutants. Land Contamination & Reclamation, 8, 175–187.
Smith, R. L., Repert, D. A., Barber, L. B., & LeBlanc, D. R. (2013). Long-term groundwater contamination after source removal—the role of sorbed carbon and nitrogen on the rate of reoxygenation of a treated-wastewater plume on Cape Cod, MA, USA. Chemical Geology, 337, 38–47.
Sun, Y., Zhang, D., & Wang, Z.-W. (2017). The potential of using biological nitrogen removal technique for stormwater treatment. Ecological Engineering, 106, 482–495.
Suzuki, T., Moribe, M., Oyama, Y., & Niinae, M. (2012). Mechanism of nitrate reduction by zero-valent iron: equilibrium and kinetics studies. Chemical Engineering Journal, 183, 271–277.
Tsitonaki, A., Petri, B., Crimi, M., MosbÆK, H., Siegrist, R. L., & Bjerg, P. L. (2010). In situ chemical oxidation of contaminated soil and groundwater using persulfate: a review. Critical Reviews in Environmental Science and Technology, 40, 55–91.
Wang, J., & Chu, L. (2016). Biological nitrate removal from water and wastewater by solid-phase denitrification process. Biotechnology Advances, 34, 1103–1112.
Wang, X., Cong, S., Wang, P., Ma, J., Liu, H., & Ning, P. (2017a). Novel green micelles Pluronic F-127 coating performance on nano zero-valent iron: enhanced reactivity and innovative kinetics. Separation and Purification Technology, 174, 174–182.
Wang, Z., Fei, X., He, S., Huang, J., & Zhou, W. (2017b). Comparison of heterotrophic and autotrophic denitrification processes for treating nitrate-contaminated surface water. Science of the Total Environment, 579, 1706–1714.
Wu, Y., Li, Y., Hui, L., Tan, Y., & Jin, S. (2009). Effects of ethanol on benzene degradation under denitrifying conditions. Bulletin of Environmental Contamination and Toxicology, 82, 145–152.
Zhang, S., Mao, G., Crittenden, J., Liu, X., & Du, H. (2017). Groundwater remediation from the past to the future: a bibliometric analysis. Water Research, 119, 114–125.
Zhu, H., Jia, Y., Wu, X., & Wang, H. (2009). Removal of arsenic from water by supported nano zero-valent iron on activated carbon. Journal of Hazardous Materials, 172, 1591–1596.
Acknowledgments
The authors gratefully acknowledge the financial support by the National Natural Science Foundation of China (No. 41502240), the Natural Science Basic Research Plan in Shaanxi Province of China (No. 2017JM4005), the Fundamental Research Funds for the Central Universities (No. 3102017zy056), the Key Laboratory of Groundwater Contamination and Remediation, China Geological Survey (CGS) & Hebei Province (No.KF201610), and the Seed Foundation of Innovation and Creation for Graduate Students in Northwestern Polytechnical University (No. Z2017192).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Hu, S., Wu, Y., Zhang, Y. et al. Nitrate Removal from Groundwater by Heterotrophic/Autotrophic Denitrification Using Easily Degradable Organics and Nano-Zero Valent Iron as Co-Electron Donors. Water Air Soil Pollut 229, 56 (2018). https://doi.org/10.1007/s11270-018-3713-5
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-018-3713-5