Bioprocess and Biosystems Engineering

, Volume 38, Issue 7, pp 1373–1380 | Cite as

N2O production in the FeII(EDTA)-NO reduction process: the effects of carbon source and pH

Original Paper


Chemical absorption–biological reduction (BioDeNOx), which uses FeII(EDTA) as a complexing agent for promoting the mass transfer efficiency of NO from gas to water, is a promising technology for removing nitric oxide (NO) from flue gases. The carbon source and pH are important parameters for FeII(EDTA)-NO (the production of absorption) reduction and N2O emissions from BioDeNOx systems. Batch tests were performed to evaluate the effects of four different carbon sources (i.e., methanol, ethanol, sodium acetate, and glucose) on FeII(EDTA)-NO reduction and N2O emissions at an initial pH of 7.2 ± 0.2. The removal efficiency of FeII(EDTA)-NO was 93.9 %, with a theoretical rate of 0.77 mmol L−1 h−1 after 24 h of operation. The highest N2O production was 0.025 mmol L−1 after 3 h when glucose was used as the carbon source. The capacities of the carbon sources to enhance the activity of the FeII(EDTA)-NO reductase enzyme decreased in the following order based on the C/N ratio: glucose > ethanol > sodium acetate > methanol. Over the investigated pH range of 5.5–8.5, the FeII(EDTA)-NO removal efficiency was highest at a pH of 7.5, with a theoretical rate of 0.88 mmol L−1 h−1. However, the N2O production was lowest at a pH of 8.5. The primary effect of pH on denitrification resulted from the inhibition of nosZ in acidic conditions.


Nitrous oxide FeII(EDTA)-NO Carbon source pH Denitrification 


  1. 1.
    Flanagan WP, Apel WA, Barnes JM, Lee BD (2002) Development of gas phase bioreactors for the removal of nitrogen oxides from synthetic flue gas streams. Fuel 81:1953–1961CrossRefGoogle Scholar
  2. 2.
    Zhou Z, Jing G, Zhou Q (2013) Enhanced NOx removal from flue gas by an integrated process of chemical absorption coupled with two-stage biological reduction using immobilized microorganisms. Process Saf Environ Prot 91:325–332CrossRefGoogle Scholar
  3. 3.
    Chen J, Dai QZ, Qian HF, Jiang YF, Chen JM (2013) Nitric oxide enhanced reduction in a rotating drum biofilter coupled with absorption by FeII(EDTA). J Chem Technol Biot 88:579–584CrossRefGoogle Scholar
  4. 4.
    Jiang R, Huang S, Chow AT, Yang J (2009) Nitric oxide removal from flue gas with a biotrickling filter using Pseudomonas putida. J Hazard Mater 164:432–441CrossRefGoogle Scholar
  5. 5.
    Zhang SH, Cai LL, Mi XH, Jiang JL, Li W (2008) NOx removal from simulated flue gas by chemical absorption-biological reduction integrated approach in a biofilter. Environ Sci Technol 42:3814–3820CrossRefGoogle Scholar
  6. 6.
    Gao L, Mi XH, Zhou Y, Li W (2011) A pilot study on the regeneration of ferrous chelate complex in NOx scrubber solution by a biofilm electrode reactor. Bioresour Technol 102:2605–2609CrossRefGoogle Scholar
  7. 7.
    Lemaire R, Meyer R, Taske A, Crocetti GR, Keller J, Yuan ZG (2006) Identifying causes for N2O accumulation in a lab-scale sequencing batch reactor performing simultaneous nitrification, denitrification and phosphorus removal. J Biotechnol 122:62–72CrossRefGoogle Scholar
  8. 8.
    Li N, Zhang Y, Li Y, Chen M, Dong X, Zhou J (2013) Reduction of Fe(II) EDTA-NO using Paracoccus denitrificans and changes of Fe(II) EDTA in the system. J Chem Technol Biotechnol 88:311–316CrossRefGoogle Scholar
  9. 9.
    Niu H, Leung D (2010) A review on the removal of nitrogen oxides from polluted flow by bioreactors. Environ Rev 18:175–189CrossRefGoogle Scholar
  10. 10.
    Parry ML (2007) Climate change 2007: impacts, adaptation and vulnerability: contribution of Working Group II to the fourth assessment report of the Intergovernmental Panel on Climate Change, Cambridge University PressGoogle Scholar
  11. 11.
    Kargi F (2003) Effect of carbon source on biological nutrient removal in a sequencing batch reactor. Bioresour Technol 89:89–93CrossRefGoogle Scholar
  12. 12.
    Adouani N, Lendormi T, Limousy L, Sire O (2010) Effect of the carbon source on N2O emissions during biological denitrification. Resour Conserv Recy 54:299–302CrossRefGoogle Scholar
  13. 13.
    Foley J, De Haas D, Yuan Z, Lant P (2010) Nitrous oxide generation in full-scale biological nutrient removal wastewater treatment plants. Water Res 44:831–844CrossRefGoogle Scholar
  14. 14.
    Dong X, Zhang Y, Zhou J, Chen M, Wang X, Shi Z (2013) Fe(II)EDTA-NO reduction coupled with Fe(II)EDTA oxidation by a nitrate- and Fe(III)-reducing bacterium. Bioresour Technol 138:339–344CrossRefGoogle Scholar
  15. 15.
    van der Maas P, van de Sandt T, Klapwijk B, Lens P (2003) Biological reduction of nitric oxide in aqueous Fe(II)EDTA solutions. Biotechnol Progr 19:1323–1328CrossRefGoogle Scholar
  16. 16.
    Dong X, Zhang Y, Zhou J, Chen M, Wang X, Shi Z (2013) Fe(II)EDTA–NO reduction coupled with Fe(II)EDTA oxidation by a nitrate- and Fe(III)-reducing bacterium. Bioresour Technol 138:339–344CrossRefGoogle Scholar
  17. 17.
    Metcalf L, Eddy HP, Tchobanoglous G (1972) Wastewater engineering: treatment, disposal, and reuse, McGraw-HillGoogle Scholar
  18. 18.
    Zhang SH, Mi XH, Cai LL, Jiang JL, Li W (2008) Evaluation of complexed NO reduction mechanism in a chemical absorption-biological reduction integrated NO(x) removal system. Appl Microbiol Biot 79:537–544CrossRefGoogle Scholar
  19. 19.
    Hagman M, Nielsen JL, Nielsen PH, Jansen JL (2008) Mixed carbon sources for nitrate reduction in activated sludge-identification of bacteria and process activity studies. Water Res 42:1539–1546CrossRefGoogle Scholar
  20. 20.
    Li QH, Li P, Zhu PP, Wu JH, Liang SZ (2008) Effects of exogenous organic carbon substrates on nitrous oxide emissions during the denitrification process of sequence batch reactors. Environ Eng Sci 25:1221–1228CrossRefGoogle Scholar
  21. 21.
    Chandrashekhar B, Pai P, Morone A, Sahu N, Pandey RA (2013) Reduction of NOx in Fe-EDTA and Fe-NTA solutions by an enriched bacterial population. Bioresour Technol 130:644–651CrossRefGoogle Scholar
  22. 22.
    Srinandan CS, D’souza G, Srivastava N, Nayak BB, Nerurkar AS (2012) Carbon sources influence the nitrate removal activity, community structure and biofilm architecture. Bioresource Technol 117:292–299CrossRefGoogle Scholar
  23. 23.
    Hu Z, Zhang J, Li S, Xie H (2013) Impact of carbon source on nitrous oxide emission from anoxic/oxic biological nitrogen removal process and identification of its emission sources. Environ Sci Pollut Res Int 20:1059–1069CrossRefGoogle Scholar
  24. 24.
    Li C, Zhang J, Liang S, Ngo HH, Guo WS, Zhang YY, Zou YN (2013) Nitrous oxide generation in denitrifying phosphorus removal process: main causes and control measures. Environ Sci Pollut R 20:5353–5360CrossRefGoogle Scholar
  25. 25.
    Vonschulthess R, Kuhni M, Gujer W (1995) Release of nitric and nitrous oxides from denitrifying activated sludge. Water Res 29:215–226CrossRefGoogle Scholar
  26. 26.
    Gambardella F, Alberts MS, Winkelman JGM, Heeres EJ (2005) Experimental and modeling studies on the absorption of NO in aqueous ferrous EDTA solutions. Ind Eng Chem Res 44:4234–4242CrossRefGoogle Scholar
  27. 27.
    Kampschreur MJ, Temmink H, Kleerebezem R, Jetten MSM, van Loosdrecht MCM (2009) Nitrous oxide emission during wastewater treatment. Water Res 43:4093–4103CrossRefGoogle Scholar
  28. 28.
    Van Den Heuvel RN, Bakker SE, Jetten MSM, Hefting MM (2011) Decreased N2O reduction by low soil pH causes high N2O emissions in a riparian ecosystem. Geobiology 9:294–300CrossRefGoogle Scholar
  29. 29.
    Pan YT, Ye L, Ni BJ, Yuan ZG (2012) Effect of pH on N2O reduction and accumulation during denitrification by methanol utilizing denitrifiers. Water Res 46:4832–4840CrossRefGoogle Scholar
  30. 30.
    Saleh-Lakha S, Shannon KE, Henderson SL, Goyer C, Trevors JT, Zebarth BJ, Burton DL (2009) Effect of pH and temperature on denitrification gene expression and activity in Pseudomonas mandelii. Appl Environ Microbiol 75:3903–3911CrossRefGoogle Scholar
  31. 31.
    Law Y, Lant P, Yuan ZG (2011) The effect of pH on N2O production under aerobic conditions in a partial nitritation system. Water Res 45:5934–5944CrossRefGoogle Scholar
  32. 32.
    Yang LC, Wang XL, Funk TL (2014) Strong influence of medium pH condition on gas-phase biofilter ammonia removal, nitrous oxide generation and microbial communities. Bioresour Technol 152:74–79CrossRefGoogle Scholar
  33. 33.
    Okabe S, Oshiki M, Takahashi Y, Satoh H (2011) N2O emission from a partial nitrification-anammox process and identification of a key biological process of N2O emission from anammox granules. Water Res 45:6461–6470CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  1. 1.Engineering Research Center of the Ministry of Education for Bioconversion and BiopurificationZhejiang University of TechnologyHangzhouPeople’s Republic of China
  2. 2.College of Biological and Environmental EngineeringZhejiang University of TechnologyHangzhouPeople’s Republic of China

Personalised recommendations