Enhanced gaseous chlorobenzene removal and its microbial mechanism through innovative modified packings coupled with magnetic field in a biotrickling filter

Abstract

Effective treatment of chlorobenzene (CB)-contaminated waste air is crucial, although biological methods are often constrained by mass transfer limitations and biodegradability. This study presents an innovative two-phase partitioning biotrickling filter coupled with magnetic bioenhancement, employing newly developed non-aqueous phase (silicone oil) immobilized polyurethane foams encapsulated in magnetically modified polyhedral hollow spheres. The removal efficiency of chlorobenzene (CB) improved by 15.6% in compared to the immobilized non-aqueous phase (INAPs) group, and by 37.2% in comparison to the control group at the inlet concentration of 150 mg/m³ with a residence time of 60 s. INAPs enhanced CB mass transfer, with kinetic analysis revealing further improvement induced by the magnetic field (MF). INAPs also promoted the secretion of extracellular polymers (EPS) by 26.8%, with enhanced secretion of loosely/tightly bound EPS promoting resistance to environmental stress. Microbial activity was optimized through INAPs that reduce substrate inhibition, with MF providing further microbial activation. The positively associated effects of INAP and MF on the microbial community was observed to lay the foundation for the positive enhancement of the combination. Overall, this study provides theoretical and technical support for the feasible and efficient treatment of industrial chlorinated volatile organic compounds.

Graphical abstract

Keywords

VOCs / Biological enhancement / Mass transfer / Microbial activity

Highlight

	● A modified packing for associated bioaugmentations was innovatively designed.
	● Magnetic field further improved mass transfer based on two-phase partitioning system.
	● Induced loosely/tightly bound EPS secretion enhanced environmental stress resistance.
	● Nonaqueous phases and magnetic fields exhibited positively associated effects.

References

[1] Amin M M, Rahimi A, Bina B, Nourmoradi H, Hassanvand M S, Mohammadi-Moghadam F, Norouzi S, Heidari M. (2017). Biodegradation of n-hexane as single pollutant and in a mixture with BTEX in a scoria/compost-based biofilter. Process Safety and Environmental Protection, 107: 508–517

[2] Bradford M M. (1976). A rapid and sensitive method for the quantitation of microgram quantities of protein utilizing the principle of protein-dye binding. Analytical Biochemistry, 72(1−2): 248–254

[3] Chakraborty P, Kumar A (2019). The extracellular matrix of mycobacterial biofilms: could we shorten the treatment of mycobacterial infections? Microbial Cell, 6(2): 105–122

[4] Chaudhary P, Padhi S K, Pattanaik L, Dikshit P K. (2025). Recent advances in treating volatile organic compounds from waste gas streams: the potential of anoxic/anaerobic bioreactors, parameters affecting their performance and future perspectives. Biomass Conversion and Biorefinery, 15(11): 16383–16408

[5] Chen D Z, Qiu J F, Sun H M, Liu Y T, Ye J X, Chen J M, Lu L C. (2024). Enhanced chlorobenzene removal by internal magnetic field through initial cell adhesion and biofilm formation. Applied Microbiology and Biotechnology, 108(1): 159

[6] Chen D Z, Zhao X Y, Miao X P, Chen J, Ye J X, Cheng Z W, Zhang S H, Chen J M. (2018). A solid composite microbial inoculant for the simultaneous removal of volatile organic sulfide compounds: preparation, characterization, and its bioaugmentation of a biotrickling filter. Journal of Hazardous Materials, 342: 589–596

[7] de Jesús Montoya-Rosales J, Palomo-Briones R, Celis L B, Etchebehere C, Cházaro-Ruiz L F, Escobar-Barrios V, Razo-Flores E. (2022). Coping with mass transfer constrains in dark fermentation using a two-phase partitioning bioreactor. Chemical Engineering Journal, 445: 136749

[8] Deng Y, Yang G F, Lens P N L, He Y X, Qie L, Shen X Y, Chen J M, Cheng Z W, Chen D Z. (2023). Enhanced removal of mixed VOCs with different hydrophobicities by tween 20 in a biotrickling filter: kinetic analysis and biofilm characteristics. Journal of Hazardous Materials, 450: 131063

[9] Elimian E A, Kiki C, Amenaghawon A N, Djellabi R. (2025). Biofiltration as a sustainable approach for the treatment of hydrophobic volatile organic compounds: improvement strategies and integrated systems. Journal of Water Process Engineering, 69: 106726

[10] Faraji A R, Khoramdareh N B, Falahati F, Jafari S, Monfared S A, Faghih A. (2023). Superparamagnetic Mn-Fe alloy composite derived from cross-bindered of chitosan/rice husk waste/iron aluminate spinel hercynite for rapid catalytic detoxification of aflatoxin B1: structure, performance and synergistic mechanism. International Journal of Biological Macromolecules, 234: 123709

[11] HanM FWangCFuY (2018). Treatment of hydrophobic volatile organic compounds using two-liquid phase biofilters. Science of the Total Environment, 640–641: 640–641

[12] Hernandez M, Quijano G, Thalasso F, Daugulis A J, Villaverde S, Munoz R. (2010). A comparative study of solid and liquid non-aqueous phases for the biodegradation of hexane in two-phase partitioning bioreactors. Biotechnology and Bioengineering, 106(5): 731–740

[13] Jia H Q, Xing Y, Zhang L G, Zhang W B, Wang J Q, Zhang H, Su W. (2023). Progress of catalytic oxidation of typical chlorined volatile organic compounds (CVOCs): a review. Science of the Total Environment, 865: 161063

[14] Krsmanovic M, Biswas D, Ali H, Kumar A, Ghosh R, Dickerson A K. (2021). Hydrodynamics and surface properties influence biofilm proliferation. Advances in Colloid and Interface Science, 288: 102336

[15] Łebkowska M, Narożniak-Rutkowska A, Pajor E. (2013). Effect of a static magnetic field of 7mT on formaldehyde biodegradation in industrial wastewater from urea–formaldehyde resin production by activated sludge. Bioresource Technology, 132: 78–83

[16] Li J R, Li D Y., Liang D B, Wu Y D, Zhu Y H, Du L Z, Yin M C, Geng Y X, Wu Y S, Li J. (2024). Static magnetic fields enhance microbial aggregation and adhesion to promote aerobic granulation. Chemical Engineering Journal, 489: 151392

[17] Li Q, Tang Z Q, Ou Yang D, Zhang J H, Chen J M, Chen D Z. (2023a). Abatement of binary gaseous chlorinated VOC by biotrickling filter: performance, interactions, and microbial community. Chemosphere, 313: 137542

[18] Li Q, Zhang K P, Yang L C, Lu L C, Kong X W, Zhao X Y, Chen J M, Chen D Z. (2023b). Novel magnetic non-aqueous phase liquid with superior recyclability for efficient and sustainable removal of gaseous n-hexane using two-phase partitioning bioreactor. Journal of Cleaner Production, 430: 139457

[19] Li X Y, Yang S F. (2007). Influence of loosely bound extracellular polymeric substances (EPS) on the flocculation, sedimentation and dewaterability of activated sludge. Water Research, 41(5): 1022–1030

[20] Lu L C, Dong D, Yeung M, Sun Z Q, Xi J Y. (2022). Sustaining low pressure drop and homogeneous flow by adopting a fluidized bed biofilter treating gaseous toluene. Chemosphere, 291: 132951

[21] Lu L C, Fang Y D, Zhang W X, Qi Q, Ju T, Chen J M, Chen D Z. (2024). Biofilm regulation through biological autocrine signaling molecules and its deuterogenic benefits on gaseous dichloromethane degradation. Chemical Engineering Journal, 495: 153585

[22] Lu L C, Ju T, Fang Y D, Hu J T, Sun Z Q, Cheng Z W, Li Q, Chen J M, Chen D Z. (2025). Efficient prediction of gaseous n-hexane removal in two-phase partitioning bioreactors with silicone oil based on the mechanism and kinetic models. Journal of Environmental Sciences, 154: 729–740

[23] Lu Y, Wang X M, Liu W P, Li E Z, Cheng F Q, Miller J D. (2019). Dispersion behavior and attachment of high internal phase water-in-oil emulsion droplets during fine coal flotation. Fuel, 253: 273–282

[24] Ma W F, Lian J R, Rene E R, Zhang P Y, Liu X. (2023). Enhanced thyroxine removal from micro-polluted drinking water resources in a bio-electrochemical reactor amended with TiO₂@GAC particles: efficiency, mechanism and energy consumption. Environmental Research, 237: 116949

[25] Marycz M, Brillowska-Dąbrowska A, Muñoz R, Gębicki J. (2022). A state of the art review on the use of fungi in biofiltration to remove volatile hydrophobic pollutants. Reviews in Environmental Science and Bio/Technology, 21(1): 225–246

[26] Meng F, Yang A Q, Zhang G M, Wang H Y. (2017). Effects of dissolved oxygen concentration on photosynthetic bacteria wastewater treatment: pollutants removal, cell growth and pigments production. Bioresource Technology, 241: 993–997

[27] MengH SChenZ JWeiWXuJDuanH RZhengMNiB J (2025). Magnetic hydrochar for sustainable wastewater management. npj Materials Sustainability, 3(1): 7

[28] Mishra B, Kallem P, Yadavalli R, Mandal S K, Reddy C N, Sumithra B, Lakshmayya N S V, Banat F. (2025). Industrial wastewater treatment using extracellular polymer substances/bioflocculants: a review. Applied Water Science, 15(3): 58

[29] Muangchinda C, Pinyakong O. (2024). Enrichment of LDPE-degrading bacterial consortia: community succession and enhanced degradation efficiency through various pretreatment methods. Scientific Reports, 14(1): 28795

[30] Pechaud Y, Derlon N, Queinnec I, Bessiere Y, Paul E. (2024). Modelling biofilm development: the importance of considering the link between EPS distribution, detachment mechanisms and physical properties. Water Research, 250: 120985

[31] Qu M M, Zheng Y, Cheng Z W, Shi Y, Wang W J, Wu X M, Chen J M. (2025). Mechanism of chlorobenzene removal in biotrickling filter enhanced by non-thermal plasma: insights from biodiversity and functional gene perspectives. Bioresource Technology, 418: 131931

[32] Raheja Y, Sharma P, Gaur P, Gaur V K, Srivastava J K. (2025). Advancing bioremediation: biosurfactants as catalysts for sustainable remediation. Biodegradation, 36(3): 33

[33] Ren Y, Yu G, Shi C P, Liu L M, Guo Q, Han C, Zhang D, Zhang L, Liu B X, Gao H. . (2022). Majorbio cloud: a one‐stop, comprehensive bioinformatic platform for multiomics analyses. iMeta, 1(2): e12

[34] RosenbergMKjellebergS. (1986). Hydrophobic interactions: role in bacterial adhesion. In: Marshall K C, ed. Advances in Microbial Ecology. New York: Springer, 353–393.

[35] Shastri A, Gore P M, Kandasubramanian B. (2024). Engineering superhydrophobicity: a survey of coating techniques for silicone-based oil–water separation membranes. Environmental Science and Pollution Research, 31(29): 41854–41872

[36] Shen L, Cheng J J, Wang J J, Cui L L, Zhang Y J, Liao W Q, Liu Z R, Zhou H, Wu X L, Li J K. . (2022). Comparison of extraction methods for extracellular polymeric substances (EPS) and dynamic characterization of EPS from sessile microorganisms during pyrite bioleaching. Journal of Environmental Chemical Engineering, 10(3): 107922

[37] Shirkosh M, Hojjat Y, Mardanpour M M. (2022). Boosting microfluidic microbial fuel cells performance via investigating electron transfer mechanisms, metal-based electrodes, and magnetic field effect. Scientific Reports, 12(1): 7417

[38] Sun L, Li M F, Gu J N, Li Y F, Liu J Z, Li Y, Li M C. (2023). High-zeta-potential accelerates interface charge transfer in lithium anodes via MXene-graphdiyne heterojunction layers. Chemical Engineering Journal, 469: 144014

[39] Tahon G, Tytgat B, Lebbe L, Carlier A, Willems A. (2018). Abditibacterium utsteinense sp. nov., The first cultivated member of candidate phylum FBP, isolated from ice-free Antarctic soil samples. Systematic and Applied Microbiology, 41(4): 279–290

[40] van den Oever A E M, Puricelli S, Costa D, Thonemann N, Lavigne Philippot M, Messagie M. (2024). Dataset with updated ozone depletion characterization factors for life cycle impact assessment. Data in Brief, 57: 111103

[41] Wang C, Xi J, Hu H, Yao Y. (2009). Stimulative effects of ozone on a biofilter treating gaseous chlorobenzene. Environmental Science & Technology, 43(24): 9407–9412

[42] Wang H L, Sun S M, Nie L, Zhang Z S, Li W P, Hao Z P. (2023). A review of whole-process control of industrial volatile organic compounds in China. Journal of Environmental Sciences, 123: 127–139

[43] Wei Z, Niu S, Wei Y, Liu Y, Xu Y X, Yang Y H, Zhang P, Zhou Q Q, Wang J J. (2024). The role of extracellular polymeric substances (EPS) in chemical-degradation of persistent organic pollutants in soil: a review. Science of the Total Environment, 912: 168877

[44] Wu P, Li G Y, He Y F, Luo D, Li L, Guo J, Ding P, Yang F. (2020). High-efficient and sustainable biodegradation of microcystin-LR using Sphingopyxis sp. YF1 immobilized Fe₃O₄@chitosan. Colloids and Surfaces B: Biointerfaces, 185: 110633

[45] Wu X, Lin Y, Wang Y Y, Dai M, Wu S H, Li X, Yang C P. (2024). Chemical structure of hydrocarbons significantly affects removal performance and microbial responses in gas biotrickling filters. Bioresource Technology, 398: 130480

[46] Wu X, Lin Y, Wang Y Y, Wu S H, Li X, Yang C P. (2022). Enhanced removal of hydrophobic short-chain n-alkanes from gas streams in biotrickling filters in presence of surfactant. Environmental Science & Technology, 56(14): 10349–10360

[47] Xie Y B, Wang X Q, Ning P, Wang L L, Ma Y X, Li Y, Cao R, Zhang H, Li X, Xu B W. (2023). Magnetic field assisted enhancement of electronic metal-support interactions in Fe_xCu_y@TiO_2-δ catalysts for arsine catalytic oxidation. Journal of Cleaner Production, 398: 136628

[48] Xing F H, Zhang H, Zhao H S, Sun B B, Wang T, Guo K Y, Dong K D, Gu S Q, Wang L Y. (2024). Novel insights into intrinsic mechanisms of magnetic field on long-term performance of anaerobic ammonium oxidation process. Bioresource Technology, 402: 130839

[49] Xing L L, Yang J X, Zhang Y Y, Ni B J, Yang C, Yuan C Y, Li A. (2022). Model-based evaluation of the impacts of aeration on tightly bound and loosely bound extracellular polymeric substance production under non-steady-state conditions. Science of the Total Environment, 852: 158566

[50] Xu D Y, Li G, Dong Y L, Wang Q W, Zhang J, Zhang G M, Lv L Y, Xia Y G, Ren Z J, Wang P F. (2023). Magnetic-field-induced simultaneous charge separation and oxygen transfer in photocatalytic oxygen activation for algae inactivation. Journal of Hazardous Materials, 446: 130693

[51] Yang Y, Zhang Z F, Zhang L, Song F F, Ren Y, Zhang X, Zhang J J, Liew R K, Foong S Y, Chong W W F. . (2023). Recent advances in the control of volatile organic compounds emissions from indoor wood-based panels: a comprehensive review. Science of the Total Environment, 884: 163741

[52] You J P, Ye L, Kong X W, Duan Y Q, Zhao J K, Chen J M, Chen D Z. (2023). Efficient biodechlorination at the Fe₃O₄-based silicone powder modified chlorobenzene-affinity anode. Journal of Hazardous Materials, 457: 131794

[53] Yu L, Bai J H, Huang L B, Zhang G L, Wang W, Wang X, Yu Z B. (2022a). Carbon-rich substrates altered microbial communities with indication of carbon metabolism functional shifting in a degraded salt marsh of the Yellow River Delta, China. Journal of Cleaner Production, 331: 129898

[54] Yu Q H, Liu G T, Shi J H, Wen T, Li L. (2022b). Magnetic-activated carbon composites derived from sludge and steel converter slag for wastewater treatment. Journal of Environmental Chemical Engineering, 10(5): 108553

[55] Zamir S M, Rene E R, Veiga M C, Kennes C. (2023). Comparative assessment of the performance of one- and two-liquid phase biotrickling filters for the simultaneous abatement of gaseous mixture of methanol, α-pinene, and hydrogen sulfide. Chemosphere, 341: 140022

[56] Zhang H, Zhang C X, Han Q. (2023). Mechanisms of bacterial inhibition and tolerance around cold atmospheric plasma. Applied Microbiology and Biotechnology, 107(17): 5301–5316

[57] Zhou H H, Xuanyuan X W, Lv X W, Wang J, Feng K, Chen C, Ma J, Xing D F. (2023). Mechanisms of magnetic sensing and regulating extracellular electron transfer of electroactive bacteria under magnetic fields. Science of the Total Environment, 895: 165104

RIGHTS & PERMISSIONS

Higher Education Press 2025