Experimental Investigation and Modeling of Denitrification of Water in a Column Bioreactor Using Immobilized Microorganisms on Modified Zeolite

Document Type : Research Paper

Authors

1 Process Design and Simulation Research Center, School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran

2 Process Design and Simulation Research Centre, School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran

3 Department of Life Science Engineering, Faculty of New Science and Technologies, University of Tehran, Tehran, Iran.

4 Microbiology and Biotechnology Research Group, Research Institute of Petroleum Industry, Tehran, Iran

5 Process Design and Simulation Research Center, School of Chemical Engineering, College of Engineering, University of Tehran, Tehran, Iran.

Abstract

The effectiveness of nitrate removal was assessed in a 9.5 L packed bed column bioreactor through the evaluation of various feeding strategies and initial concentrations. The bioreactor was filled with zeolite mineral particles and initially treated with Thiobacillus denitrificans. Multiple hydraulic retention times were investigated to determine the efficiency of nitrate removal. The results demonstrate that the designed bioreactor is capable of achieving an 87% reduction in nitrate levels within a three-hour timeframe. This indicates that the bioreactor system can effectively remove nitrate ions from water, even when the initial nitrate content is as high as 400 mg/L, which exceeds the standard limit of 45 mg/L. The computational fluid dynamics (CFD) model yielded satisfactory results, confirming the effectiveness of the bioreactor design. It revealed that the optimal length of the bioreactor is suitable for influents containing 400 mg/L of nitrate. However, for influents with lower nitrate concentrations or when employing lower hydraulic retention times (HRTs), the bioreactor can be constructed with shorter heights. This CFD model can serve as a valuable tool for future studies, particularly in scaling up the bioreactor system.

Keywords

Main Subjects


[1] Jensen VB, Darby JL, Seidel C, Gorman C. Nitrate in potable water supplies: alternative
management strategies. Critical Reviews in Environmental Science and Technology.
2014;44(20):2203-86. https://doi.org/10.1080/10643389.2013.828272
[2] Kancherla R, Kumar VR, Prabhaker Reddy G, Sridhar S. Nitrate removal studies on
polyurea membrane using nanofiltration system–membrane characterization and model
development. Chemical Product and Process Modeling. 2020;17(1):81-99.
https://doi.org/10.1515/cppm-2020-0041
[3] Maheswari P, Sheik AG, Tejaswini E, Ambati SR. Nested control loop configuration for a
three-stage biological wastewater treatment process. Chemical Product and Process
Modeling. 2020;16(2):87-100. https://doi.org/10.1515/cppm-2020-0035
[4] Tejaswini E, Uday Bhaskar Babu G, Seshagiri Rao A. Effect of temperature on effluent
quality in a biological wastewater treatment process. Chemical Product and Process
Modeling. 2019;15(1):20190018. https://doi.org/10.1515/cppm-2019-0018
[5] Rajab Beigy M, Rasekh B, Yazdian F, Aminzadeh B, Shekarriz M. High nitrate removal by
starch‐stabilized Fe0 nanoparticles in aqueous solution in a controlled system. Engineering
in Life Sciences. 2018;18(3):187-95. https://doi.org/10.1002/elsc.201700127
[6] Rajab Beiki M, Yazdian F, Rasekh B, Rashedi H, Darzian Rostami A. Effect of metal
nanoparticles on biological denitrification process: a review. Journal of Applied
Biotechnology Reports. 2016;3(1):353-8.
[7] Rezvani F, Sarrafzadeh M-H, Ebrahimi S, Oh H-M. Nitrate removal from drinking water
with a focus on biological methods: a review. Environmental Science and Pollution
Research. 2019; 26:1124-41.
[8] Sharma SK, Sobti RC. Nitrate removal from ground water: a review. E-Journal of
Chemistry. 2012;9(4):1667-75. https://doi.org/10.1155/2012/154616
[9] Ashok V, Hait S. Remediation of nitrate-contaminated water by solid-phase denitrification
process—a review. Environmental Science and Pollution Research. 2015; 22:8075-93.
https://doi.org/10.1007/s11356-015-4334-9
[10] Sierra-Alvarez R, Beristain-Cardoso R, Salazar M, Gómez J, Razo-Flores E, Field JA.
Chemolithotrophic denitrification with elemental sulfur for groundwater treatment. Water
research. 2007;41(6):1253-62. https://doi.org/10.1016/j.watres.2006.12.039
[11] Zhang Z, Lei Z, He X, Zhang Z, Yang Y, Sugiura N. Nitrate removal by Thiobacillus
denitrificans immobilized on poly (vinyl alcohol) carriers. Journal of Hazardous Materials.
2009;163(2-3):1090-5. https://doi.org/10.1016/j.jhazmat.2008.07.062
[12] Zhang R-C, Chen C, Xu X-J, Lee D-J, Ren N-Q. The interaction between Pseudomonas
C27 and Thiobacillus denitrificans in the integrated autotrophic and heterotrophic
denitrification process. Science of the Total Environment. 2022; 811:152360.
https://doi.org/10.1016/j.scitotenv.2021.152360
[13] Polizzi C, Gabriel D, Munz G. Successful sulphide-driven partial denitrification: Efficiency,
stability and resilience in SRT-controlled conditions. Chemosphere. 2022; 295:133936.
https://doi.org/10.1016/j.chemosphere.2022.133936
[14] Han J, Qi X, Liang P. Improved sulfur autotrophic denitrification using supplementary
bovine serum albumin. Science of The Total Environment. 2023; 859:160147.
https://doi.org/10.1016/j.scitotenv.2022.160147
[15] Koenig A, Liu L. Autotrophic denitrification of landfill leachate using elemental Sulphur.
Water Science and Technology. 1996;34(5-6):469-76.
https://doi.org/10.1016/0273-1223(96)00680-4
[16] Koenig A, Liu L. Kinetic model of autotrophic denitrification in Sulphur packed-bed
reactors. Water research. 2001;35(8):1969-78.
https://doi.org/10.1016/S0043-1354(00)00483-8
[17] Zhang TC, Lampe DG. Sulfur: limestone autotrophic denitrification processes for treatment
of nitrate-contaminated water: batch experiments. Water Research. 1999;33(3):599-608.
https://doi.org/10.1016/S0043-1354(98)00281-4
[18] Wang H, Qu J. Combined bio electrochemical and sulfur autotrophic denitrification for
drinking water treatment. Water Research. 2003;37(15):3767-75.
https://doi.org/10.1016/S0043-1354(03)00249-5
[19] Flere JM, Zhang TC. Nitrate removal with sulfur-limestone autotrophic denitrification
processes. Journal of Environmental Engineering. 1999;125(8):721-9.
https://doi.org/10.1061/(ASCE)0733-9372(1999)125:8(721)
[20] Wallenstein MD, McNulty S, Fernandez IJ, Boggs J, Schlesinger WH. Nitrogen fertilization
decreases forest soil fungal and bacterial biomass in three long-term experiments. Forest
Ecology and Management. 2006;222(1-3):459-68.
https://doi.org/10.1016/j.foreco.2005.11.002
[21] Chen Y, Su Y, Zheng X, Chen H, Yang H. Alumina nanoparticles-induced effects on
wastewater nitrogen and phosphorus removal after short-term and long-term exposure.
Water research. 2012;46(14):4379-86. https://doi.org/10.1016/j.watres.2012.05.042
[22] Kurt M, Dunn I, Bourne J. Biological denitrification of drinking water using autotrophic
organisms with H2 in a fluidized‐bed biofilm reactor. Biotechnology and bioengineering.
1987;29(4):493-501. https://doi.org/10.1002/bit.260290414
[23] Montalvo S, Guerrero L, Borja R, Sánchez E, Milán Z, Cortés I, et al. Application of natural
zeolites in anaerobic digestion processes: A review. Applied Clay Science. 2012; 58:125-
33. https://doi.org/10.1016/j.clay.2012.01.013
[24] Chu L, Wang J. Denitrification performance and biofilm characteristics using biodegradable
polymers PCL as carriers and carbon source. Chemosphere. 2013;91(9):1310-6.
https://doi.org/10.1016/j.chemosphere.2013.02.064
[7] Rezvani F, Sarrafzadeh M-H, Ebrahimi S, Oh H-M. Nitrate removal from drinking water
with a focus on biological methods: a review. Environmental Science and Pollution
Research. 2019; 26:1124-41.
[8] Sharma SK, Sobti RC. Nitrate removal from ground water: a review. E-Journal of
Chemistry. 2012;9(4):1667-75. https://doi.org/10.1155/2012/154616
[9] Ashok V, Hait S. Remediation of nitrate-contaminated water by solid-phase denitrification
process—a review. Environmental Science and Pollution Research. 2015; 22:8075-93.
https://doi.org/10.1007/s11356-015-4334-9
[10] Sierra-Alvarez R, Beristain-Cardoso R, Salazar M, Gómez J, Razo-Flores E, Field JA.
Chemolithotrophic denitrification with elemental sulfur for groundwater treatment. Water
research. 2007;41(6):1253-62. https://doi.org/10.1016/j.watres.2006.12.039
[11] Zhang Z, Lei Z, He X, Zhang Z, Yang Y, Sugiura N. Nitrate removal by Thiobacillus
denitrificans immobilized on poly (vinyl alcohol) carriers. Journal of Hazardous Materials.
2009;163(2-3):1090-5. https://doi.org/10.1016/j.jhazmat.2008.07.062
[12] Zhang R-C, Chen C, Xu X-J, Lee D-J, Ren N-Q. The interaction between Pseudomonas
C27 and Thiobacillus denitrificans in the integrated autotrophic and heterotrophic
denitrification process. Science of the Total Environment. 2022; 811:152360.
https://doi.org/10.1016/j.scitotenv.2021.152360
[13] Polizzi C, Gabriel D, Munz G. Successful sulphide-driven partial denitrification: Efficiency,
stability and resilience in SRT-controlled conditions. Chemosphere. 2022; 295:133936.
https://doi.org/10.1016/j.chemosphere.2022.133936
[14] Han J, Qi X, Liang P. Improved sulfur autotrophic denitrification using supplementary
bovine serum albumin. Science of The Total Environment. 2023; 859:160147.
https://doi.org/10.1016/j.scitotenv.2022.160147
[15] Koenig A, Liu L. Autotrophic denitrification of landfill leachate using elemental Sulphur.
Water Science and Technology. 1996;34(5-6):469-76.
https://doi.org/10.1016/0273-1223(96)00680-4
[16] Koenig A, Liu L. Kinetic model of autotrophic denitrification in Sulphur packed-bed
reactors. Water research. 2001;35(8):1969-78.
https://doi.org/10.1016/S0043-1354(00)00483-8
[17] Zhang TC, Lampe DG. Sulfur: limestone autotrophic denitrification processes for treatment
of nitrate-contaminated water: batch experiments. Water Research. 1999;33(3):599-608.
https://doi.org/10.1016/S0043-1354(98)00281-4
[18] Wang H, Qu J. Combined bio electrochemical and sulfur autotrophic denitrification for
drinking water treatment. Water Research. 2003;37(15):3767-75.
https://doi.org/10.1016/S0043-1354(03)00249-5
[19] Flere JM, Zhang TC. Nitrate removal with sulfur-limestone autotrophic denitrification
processes. Journal of Environmental Engineering. 1999;125(8):721-9.
https://doi.org/10.1061/(ASCE)0733-9372(1999)125:8(721)
[20] Wallenstein MD, McNulty S, Fernandez IJ, Boggs J, Schlesinger WH. Nitrogen fertilization
decreases forest soil fungal and bacterial biomass in three long-term experiments. Forest
Ecology and Management. 2006;222(1-3):459-68.
https://doi.org/10.1016/j.foreco.2005.11.002
[21] Chen Y, Su Y, Zheng X, Chen H, Yang H. Alumina nanoparticles-induced effects on
wastewater nitrogen and phosphorus removal after short-term and long-term exposure.
Water research. 2012;46(14):4379-86. https://doi.org/10.1016/j.watres.2012.05.042
[22] Kurt M, Dunn I, Bourne J. Biological denitrification of drinking water using autotrophic
organisms with H2 in a fluidized‐bed biofilm reactor. Biotechnology and bioengineering.
1987;29(4):493-501. https://doi.org/10.1002/bit.260290414
[23] Montalvo S, Guerrero L, Borja R, Sánchez E, Milán Z, Cortés I, et al. Application of natural
zeolites in anaerobic digestion processes: A review. Applied Clay Science. 2012; 58:125-
33. https://doi.org/10.1016/j.clay.2012.01.013
[24] Chu L, Wang J. Denitrification performance and biofilm characteristics using biodegradable
polymers PCL as carriers and carbon source. Chemosphere. 2013;91(9):1310-6.
https://doi.org/10.1016/j.chemosphere.2013.02.064
[25] Yamashita T, Yamamoto-Ikemoto R, Zhu J. Sulfate-reducing bacteria in a denitrification
reactor packed with wood as a carbon source. Bioresource Technology. 2011;102(3):2235-
41. https://doi.org/10.1016/j.biortech.2010.10.015
[26] Moreno-Castilla C, Bautista-Toledo I, Ferro-Garcıa M, Rivera-Utrilla J. Influence of
support surface properties on activity of bacteria immobilised on activated carbons for water
denitrification. Carbon. 2003;41(9):1743-9.
https://doi.org/10.1016/S0008-6223(03)00123-4
[27] Soy E, Pyeshkova V, Arkhypova V, Khadro B, Jaffrezic-Renault N, Sacco Jr A, et al.
Potentialities of zeolites for immobilization of enzymes in conductometric biosensors.
Сенсорна електроніка і мікросистемні технології. 2010;7(1):28-35.
https://doi.org/10.18524/1815-7459.2010.1.114008
[28] Bautista-Toledo M, Espinosa-Iglesias D, Carrasco-Marín F, Pérez-Cadenas A, MaldonadoHódar F. Influence of the physicochemical properties of inorganic supports on the activity
of immobilized bacteria for water denitrification. Journal of Environmental Management.
2015; 156:81-8. https://doi.org/10.1016/j.jenvman.2015.03.031
[29] Philippot L. Denitrifying genes in bacterial and archaeal genomes. Biochimica et biophysica
acta (BBA)-Gene structure and expression. 2002;1577(3):355-76.
https://doi.org/10.1016/S0167-4781(02)00420-7
[30] Di Capua F, Papirio S, Lens PN, Esposito G. Chemolithotrophic denitrification in biofilm
reactors. Chemical Engineering Journal. 2015; 280:643-57.
https://doi.org/10.1016/j.cej.2015.05.131
[31] Abyaneh EZ, Zarghami R, Krühne U, Grundtvig IPR, Ramin P, Mostoufi N. Mixing
assessment of an industrial anaerobic digestion reactor using CFD. Renewable Energy.
2022; 192:537-49. https://doi.org/10.1016/j.renene.2022.04.147
[32] Park J-H, Shin H-S, Lee I-S, Bae J-H. Denitrification of high NO3−-N containing
wastewater using elemental sulfur; nitrogen loading rate and N2O production.
Environmental technology. 2002;23(1):53-65.
https://doi.org/10.1080/09593332508618431
[33] Zhao Y, Feng C, Wang Q, Yang Y, Zhang Z, Sugiura N. Nitrate removal from groundwater
by cooperating heterotrophic with autotrophic denitrification in a biofilm–electrode reactor.
Journal of hazardous materials. 2011;192(3):1033-9.
https://doi.org/10.1016/j.jhazmat.2011.06.008
[34] Wan D, Liu H, Qu J, Lei P, Xiao S, Hou Y. Using the combined bioelectrochemical and
sulfur autotrophic denitrification system for groundwater denitrification. Bioresource
technology. 2009;100(1):142-8. https://doi.org/10.1016/j.biortech.2008.05.042
[35] Torrentó C, Cama J, Urmeneta J, Otero N, Soler A. Denitrification of groundwater with
pyrite and Thiobacillus denitrificans. Chemical Geology. 2010;278(1-2):80-91.
https://doi.org/10.1016/j.chemgeo.2010.09.003
[36] Carrera J, Vicent T, Lafuente F. Influence of temperature on denitrification of an industrial
high-strength nitrogen wastewater in a two-sludge system. Water Sa. 2003;29(1):11-6.
https://doi.org/10.4314/wsa.v29i1.4939
[37] Gu J-D, Qiu W, Koenig A, Fan Y. Removal of high NO3Ð concentrations in saline water
through autotrophic denitrification by the bacterium Thiobacillus denitrificans strain MP.
Water Science and Technology. 2004;49(5-6):105-12.
https://doi.org/10.2166/wst.2004.0743
[38] Shirazi L, Jamshidi E, Ghasemi M. The effect of Si/Al ratio of ZSM‐5 zeolite on its
morphology, acidity and crystal size. Crystal Research and Technology: Journal of
Experimental and Industrial Crystallography. 2008;43(12):1300-6.
https://doi.org/10.1002/crat.200800149
[39] Koenig A, Liu L. Use of limestone for pH control in autotrophic denitrification: continuous
flow experiments in pilot-scale packed bed reactors. Journal of Biotechnology.
2002;99(2):161-71. https://doi.org/10.1016/S0168-1656(02)00183-9
[40] Sahinkaya E, Kilic A, Duygulu B. Pilot and full-scale applications of sulfur-based
autotrophic denitrification process for nitrate removal from activated sludge process
effluent. Water Research. 2014; 60:210-7. https://doi.org/10.1016/j.watres.2014.04.052
[41] Kopec L, Kopec A, Drewnowski J. The application of Monod equation to denitrification
kinetics description in the moving bed biofilm reactor (MBBR). International Journal of
Environmental Science and Technology. 2019; 16:1479-86.
https://doi.org/10.1007/s13762-018-1829-1
[42] Rezvani F, Sarrafzadeh M-H. Autotrophic granulation of hydrogen consumer denitrifiers
and microalgae for nitrate removal from drinking water resources at different hydraulic
retention times. Journal of Environmental Management. 2020; 268:110674.
https://doi.org/10.1016/j.jenvman.2020.110674