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Electrocatalytic biofilm reactor for effective and energy-efficient azo dye degradation: the synergistic effect of MnOx/Ti flow-through anode and biofilm on the cathode

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Abstract

Dyeing wastewater treatment remains a challenge. Although effective, the in-series process using electrochemical oxidation as the pre- or post-treatment of biodegradation is long. This study proposes a compact dual-chamber electrocatalytic biofilm reactor (ECBR) to complete azo dye decolorization and mineralization in a single unit via anodic oxidation on a MnOx/Ti flow-through anode followed by cathodic biodegradation on carbon felts. Compared with the electrocatalytic reactor with a stainless-steel cathode (ECR-SS) and the biofilm reactor (BR), the ECBR increased the chemical oxygen demand (COD) removal efficiency by 24 % and 31 % (600 mg/L Acid Orange 7 as the feed, current of 6 mA), respectively. The COD removal efficiency of the ECBR was even higher than the sum of those of ECR-SS and BR. The ECBR also reduced the energy consumption (3.07 kWh/kg COD) by approximately half compared with ECR-SS. The advantages of the ECBR in azo dye removal were attributed to the synergistic effect of the MnOx/Ti flow-through anode and cathodic biofilms. Catalyzed by MnIV=O generated on the MnOx/Ti anode under a low applied current, azo dyes were oxidized and decolored. The intermediate products with improved biodegradability were further mineralized by the cathodic aerobic heterotrophic bacteria (non-electrochemically active) under the stimulation of the applied current. Taking advantage of the mutual interactions among the electricity, anode, and bacteria, this study provides a novel and compact process for the effective and energy-efficient treatment of azo dye wastewater.

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References

  • Ailijiang N, Chang J, Liang P, Li P, Wu Q, Zhang X, Huang X (2016). Electrical stimulation on biodegradation of phenol and responses of microbial communities in conductive carriers supported biofilms of the bioelectrochemical reactor. Bioresource Technology, 201: 1–7

    Article  CAS  Google Scholar 

  • Aravind P, Selvaraj H, Ferro S, Sundaram M (2016). An integrated (electro- and bio-oxidation) approach for remediation of industrial wastewater containing azo-dyes: understanding the degradation mechanism and toxicity assessment. Journal of Hazardous Materials, 318: 203–215

    Article  CAS  Google Scholar 

  • Bin D, Wang H, Li J, Wang H, Yin Z, Kang J, He B, Li Z (2014). Controllable oxidation of glucose to gluconic acid and glucaric acid using an electrocatalytic reactor. Electrochimica Acta, 130: 170–178

    Article  CAS  Google Scholar 

  • Bu L, Ding J, Zhu N, Kong M, Wu Y, Shi Z, Zhou S, Dionysiou D D (2019). Unraveling different mechanisms of persulfate activation by graphite felt anode and cathode to destruct contaminants of emerging concern. Applied Catalysis B: Environmental, 253: 140–148

    Article  CAS  Google Scholar 

  • Cao Z, Zhang J, Zhang J, Zhang H (2017). Degradation pathway and mechanism of Reactive Brilliant Red X-3B in electro-assisted microbial system under anaerobic condition. Journal of Hazardous Materials, 329: 159–165

    Article  CAS  Google Scholar 

  • Chacón-Patiño M L, Blanco-Tirado C, Hinestroza J P, Combariza M Y (2013). Biocomposite of nanostructured MnO2 and fique fibers for efficient dye degradation. Green Chemistry, 15(10): 2920–2928

    Article  Google Scholar 

  • Cui D, Cui M H, Liang B, Liu W Z, Tang Z E, Wang A J (2020). Mutual effect between electrochemically active bacteria (EAB) and azo dye in bio-electrochemical system (BES). Chemosphere, 239: 124787

    Article  CAS  Google Scholar 

  • Cui M H, Liu W Z, Tang Z E, Cui D (2021). Recent advancements in azo dye decolorization in bio-electrochemical systems (BESs): Insights into decolorization mechanism and practical application. Water Research, 203: 117512

    Article  CAS  Google Scholar 

  • Fang X, Yin Z, Wang H, Li J, Liang X, Kang J, He B (2015). Controllable oxidation of cyclohexane to cyclohexanol and cyclohexanone by a nano-MnOx/Ti electrocatalytic membrane reactor. Journal of Catalysis, 329: 187–194

    Article  CAS  Google Scholar 

  • Huang T, Liu L, Tao J, Zhou L, Zhang S (2018). Microbial fuel cells coupling with the three-dimensional electro-Fenton technique enhances the degradation of methyl orange in the wastewater. Environmental Science and Pollution Research International, 25(18): 17989–18000

    Article  CAS  Google Scholar 

  • Hui H, Wang H, Mo Y, Yin Z, Li J (2019). Optimal design and evaluation of electrocatalytic reactors with nano-MnOx/Ti membrane electrode for wastewater treatment. Chemical Engineering Journal, 376: 120190

    Article  CAS  Google Scholar 

  • Jen J F, Leu M F, Yang T C (1998). Determination of hydroxyl radicals in an advanced oxidation process with salicylic acid trapping and liquid chromatography. Journal of Chromatography A, 796(2): 283–288

    Article  CAS  Google Scholar 

  • Kudlich M, Hetheridge M J, Knackmuss H J, Stolz A (1999). Autoxidation reactions of different aromatic o-aminohydroxynaphthalenes that are formed during the anaerobic reduction of sulfonated azo dyes. Environmental Science & Technology, 33(6): 896–901

    Article  CAS  Google Scholar 

  • Ledakowicz S, Paździor K (2021). Recent achievements in dyes removal focused on advanced oxidation processes integrated with biological methods. Molecules (Basel, Switzerland), 26(4): 870

    Article  CAS  Google Scholar 

  • Li J, Li J, Wang H, Cheng B, He B, Yan F, Yang Y, Guo W, Ngo H H (2013). Electrocatalytic oxidation of n-propanol to produce propionic acid using an electrocatalytic membrane reactor. Chemical Communications, 49(40): 4501–4503

    Article  CAS  Google Scholar 

  • Li X, Jin X, Zhao N, Angelidaki I, Zhang Y (2017). Novel bio-electro-Fenton technology for azo dye wastewater treatment using microbial reverse-electrodialysis electrolysis cell. Bioresource Technology, 228: 322–329

    Article  CAS  Google Scholar 

  • Liang P, Wei J, Li M, Huang X (2013). Scaling up a novel denitrifying microbial fuel cell with an oxic-anoxic two stage biocathode. Frontiers of Environmental Science & Engineering, 7(6): 913–919

    Article  CAS  Google Scholar 

  • Liang S, Zhang B, Shi J, Wang T, Zhang L, Wang Z, Chen C (2018). Improved decolorization of dye wastewater in an electrochemical system powered by microbial fuel cells and intensified by micro-electrolysis. Bioelectrochemistry (Amsterdam, Netherlands), 124: 112–118

    Article  CAS  Google Scholar 

  • Liu S, Song H, Wei S, Liu Q, Li X, Qian X (2015). Effect of direct electrical stimulation on decolorization and degradation of azo dye reactive brilliant red X-3B in biofilm-electrode reactors. Biochemical Engineering Journal, 93: 294–302

    Article  CAS  Google Scholar 

  • Logan B E, Hamelers B, Rozendal R, Schröder U, Keller J, Freguia S, Aelterman P, Verstraete W, Rabaey K (2006). Microbial fuel cells: methodology and technology. Environmental Science & Technology, 40(17): 5181–5192

    Article  CAS  Google Scholar 

  • Logan B E, Rabaey K (2012). Conversion of wastes into bioelectricity and chemicals by using microbial electrochemical technologies. Science, 337(6095): 686–690

    Article  CAS  Google Scholar 

  • Lu L, Ren Z J (2016). Microbial electrolysis cells for waste biorefinery: a state of the art review. Bioresource Technology, 215: 254–264

    Article  CAS  Google Scholar 

  • Mo Y, Du M, Cui S, Wang H, Zhao X, Zhang M, Li J (2021). Simultaneously enhancing degradation of refractory organics and achieving nitrogen removal by coupling denitrifying biocathode with MnOx/Ti anode. Journal of Hazardous Materials, 402: 123467

    Article  CAS  Google Scholar 

  • Mo Y, Du M, Yuan T, Liu M, Wang H, He B, Li J, Zhao X (2020). Enhanced anodic oxidation and energy saving for dye removal by integrating O2-reducing biocathode into electrocatalytic reactor. Chemosphere, 252: 126460

    Article  CAS  Google Scholar 

  • Mo Y, Yuan T, Liu M, Du M, Wang H, He B, Li J (2019). Integrating biocathode into electrocatalytic reactor to reduce applied voltage to generate hydroxyl radicals for advanced oxidation. Journal of Chemical Technology and Biotechnology (Oxford, Oxfordshire), 94(8): 2487–2496

    Article  CAS  Google Scholar 

  • Moreira F C, Boaventura R A R, Brillas E, Vilar V J P (2017). Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Applied Catalysis B: Environmental, 202: 217–261

    Article  CAS  Google Scholar 

  • Nidheesh P V, Zhou M, Oturan M A (2018). An overview on the removal of synthetic dyes from water by electrochemical advanced oxidation processes. Chemosphere, 197: 210–227

    Article  CAS  Google Scholar 

  • O’Neill C, Lopez A, Esteves S, Hawkes F R, Hawkes D L, Wilcox S (2000). Azo-dye degradation in an anaerobic-aerobic treatment system operating on simulated textile effluent. Applied Microbiology and Biotechnology, 53(2): 249–254

    Article  Google Scholar 

  • Oturan M A, Aaron J J (2014). Advanced oxidation processes in water/wastewater treatment: principles and applications. a review. Critical Reviews in Environmental Science and Technology, 44(23): 2577–2641

    Article  CAS  Google Scholar 

  • Pazdzior K, Biliñska L, Ledakowicz S (2019). A review of the existing and emerging technologies in the combination of AOPs and biological processes in industrial textile wastewater treatment. Chemical Engineering Journal, 376: 120597

    Article  CAS  Google Scholar 

  • Ramesh M, Nagaraja H S, Rao M P, Anandan S, Huang N M (2016). Fabrication, characterization and catalytic activity of alpha-MnO2 nanowires for dye degradation of reactive black 5. Materials Letters, 172: 85–89

    Article  CAS  Google Scholar 

  • Sathishkumar K, AlSalhi M S, Sanganyado E, Devanesan S, Arulprakash A, Rajasekar A (2019). Sequential electrochemical oxidation and bio-treatment of the azo dye congo red and textile effluent. Journal of Photochemistry and Photobiology. B, Biology, 200:111655

    CAS  Google Scholar 

  • Sirés I, Brillas E, Oturan M A, Rodrigo M A, Panizza M (2014). Electrochemical advanced oxidation processes: today and tomorrow: a review. Environmental Science and Pollution Research International, 21(14): 8336–8367

    Article  Google Scholar 

  • Solanki K, Subramanian S, Basu S (2013). Microbial fuel cells for azo dye treatment with electricity generation: a review. Bioresource Technology, 131: 564–571

    Article  CAS  Google Scholar 

  • Stolz A (2001). Basic and applied aspects in the microbial degradation of azo dyes. Applied Microbiology and Biotechnology, 56(1–2): 69–80

    Article  CAS  Google Scholar 

  • Sun J, Hu Y, Li W, Zhang Y, Chen J, Deng F (2015). Sequential decolorization of azo dye and mineralization of decolorization liquid coupled with bioelectricity generation using a pH self-neutralized photobioelectrochemical system operated with polarity reversion. Journal of Hazardous Materials, 289: 108–117

    Article  CAS  Google Scholar 

  • Sun L, Mo Y, Zhang L (2022). A mini review on bio-electrochemical systems for the treatment of azo dye wastewater: state-of-the-art and future prospects. Chemosphere, 294: 133801

    Article  CAS  Google Scholar 

  • Sun Q, Li Z L, Wang Y Z, Yang C X, Chung J S, Wang A J (2016). Cathodic bacterial community structure applying the different co-substrates for reductive decolorization of Alizarin Yellow R. Bioresource Technology, 208: 64–72

    Article  CAS  Google Scholar 

  • Wang S, Qi X, Jiang Y, Liu P, Hao W, Han J, Liang P (2022). An antibiotic composite electrode for improving the sensitivity of electrochemically active biofilm biosensor. Frontiers of Environmental Science & Engineering, 16(8): 97

    Article  CAS  Google Scholar 

  • Xia X, Tokash J C, Zhang F, Liang P, Huang X, Logan B E (2013). Oxygen-reducing biocathodes operating with passive oxygen transfer in microbial fuel cells. Environmental Science & Technology, 47(4): 2085–2091

    Article  CAS  Google Scholar 

  • Xu H, Quan X, Chen L (2019). A novel combination of bioelectrochemical system with peroxymonosulfate oxidation for enhanced azo dye degradation and MnFe2O4 catalyst regeneration. Chemosphere, 217: 800–807

    Article  CAS  Google Scholar 

  • Zou H, Wang Y (2017). Azo dyes wastewater treatment and simultaneous electricity generation in a novel process of electrolysis cell combined with microbial fuel cell. Bioresource Technology, 235:167–175

    Article  CAS  Google Scholar 

  • Zuo K, Cai J, Liang S, Wu S, Zhang C, Liang P, Huang X (2014). A ten liter stacked microbial desalination cell packed with mixed ion-exchange resins for secondary effluent desalination. Environmental Science & Technology, 48(16): 9917–9924

    Article  CAS  Google Scholar 

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (No. 2020YFA0211003), the National Natural Science Foundation of China (Nos. 51978465, 21878230, and 51878646), and the Natural Science Foundation of Tianjin of China (Nos. 19JCQNJC07500 and 19JCZDJC39800).

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Correspondence to Yinghui Mo or Liang Wang.

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Highlights

• MnOx/Ti flow-through anode was coupled with the biofilm-attached cathode in ECBR.

• ECBR was able to enhance the azo dye removal and reduce the energy consumption. • MnIV=O generated on the electrified MnOx/Ti anode catalyzed the azo dye oxidation.

• Aerobic heterotrophic bacteria on the cathode degraded azo dye intermediate products.

• Biodegradation of intermediate products was stimulated under the electric field.

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Mo, Y., Sun, L., Zhang, L. et al. Electrocatalytic biofilm reactor for effective and energy-efficient azo dye degradation: the synergistic effect of MnOx/Ti flow-through anode and biofilm on the cathode. Front. Environ. Sci. Eng. 17, 49 (2023). https://doi.org/10.1007/s11783-023-1649-5

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  • DOI: https://doi.org/10.1007/s11783-023-1649-5

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