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Binary electrochemical mineralization of heterocyclic nitrogenous compounds: parametric optimization using Taguchi method and mineralization mechanism

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Abstract

The main objective of the present work was to understand the interactive behaviour of various operating parameters including concentration of pollutants during binary electrochemical mineralization of the two nitrogenous heterocyclic pollutants in the aqueous solution. Indole and pyrrole were selected as pollutants, whereas Pt/Ti was selected as anode and cathode. The effects of different operating parameters like current density, solution conductivity, initial concentration of the pollutants and time were studied. Taguchi method was used to optimize these operating parameters for obtaining the ultimate rate of degradation for the nitrogenous compounds. There were basically two responses, i.e. chemical oxygen demand (COD) degradation and specific energy consumption. These responses were maximized and minimized, respectively. At the optimum condition, removal efficiencies of pyrrole, indole and COD were found to be 46.1%, 62.4% and 61.4%, respectively. The optimum value of specific energy consumption was found to be 159.5 kWh per kg COD removed. Possible mineralization pathways are also proposed on the basis of the identified intermediates by gas chromatography coupled with mass spectroscopy. The operating cost was also calculated for the binary lab-scale treatment of the indole and pyrrole and compared with reported cost analysis for the electrochemical treatment.

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Data availability

The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.

References

  • Ahlawat R, Srivastava VC, Mall ID, Sinha S (2008) Investigation of the electrochemical treatment of cotton blue dye solutions using aluminum electrodes. Clean – Soil, Air, Water 36(10–11):863–869

    Article  CAS  Google Scholar 

  • Aravind P, Selvaraj H, Ferro S, Neelavannan GM, Sundaram M (2018) A one-pot approach: Oxychloride radicals enhanced electrochemical oxidation for the treatment of textile dye wastewater trailed by mixed salts recycling. J Clean Prod 182:246–258

    Article  CAS  Google Scholar 

  • Cañizares P, Paz R, Sáez C, Rodrigo MA (2009) Costs of the electrochemical oxidation of wastewaters: a comparison with ozonation and Fenton oxidation processes. J Environ Manag 90:410–420

    Article  Google Scholar 

  • Chauhan R, Srivastava VC (2020) Electrochemical denitrification of highly contaminated actual nitrate wastewater by Ti/RuO2 anode and iron cathode. Chem Eng J 386:122065

  • Chauhan R, Srivastava VC, Hiwarkar AD (2016) Electrochemical mineralization of chlorophenol by ruthenium oxide coated titanium electrode. J Taiwan Inst Chem Eng 69:106–117

    Article  CAS  Google Scholar 

  • Chen S, Pan H, Chang Z, Jin M, Pu H (2019) Synthesis and study of pyridine-containing sulfonated polybenzimidazole multiblock copolymer for proton exchange membrane fuel cells. Ionics (Kiel) 25:2255–2265

    Article  CAS  Google Scholar 

  • Chun D, Lim CR, Lee HS, Yoon WS, Lee TK, Kim DK (2018) Electrochemical treatment of urine by using Ti/IrO2/TiO2 electrode. J Water Process Eng 26:1–9

    Article  Google Scholar 

  • Comninellis C, Nerini A (1995) Anodic oxidation of phenol in the presence of NaCl for wastewater treatment. J Appl Electrochem 25:23–28

    Article  CAS  Google Scholar 

  • Gale RS (1967) Filtration theory with special reference to sewage sludges. Water Pollution Control 66:622–632

    Google Scholar 

  • García-Espinoza JD, Nacheva PM (2019) Effect of electrolytes on the simultaneous electrochemical oxidation of sulfamethoxazole, propranolol and carbamazepine: behaviors, by-products and acute toxicity. Environ Sci Pollut Res 26:6855–6867

    Article  Google Scholar 

  • Gonul LT, Kucuksezgin F (2012) Aliphatic and polycyclic aromatic hydrocarbons in the surface sediments from the Eastern Aegean: assessment and source recognition of petroleum hydrocarbons. Environ Sci Pollut Res 19:31–41

    Article  CAS  Google Scholar 

  • Gupta D, Chauhan R, Kumar N, Singh V, Srivastava VC, Mohanty P, Mandal TK (2020) Enhancing photocatalytic degradation of quinoline by ZnO:TiO2 mixed oxide: optimization of operating parameters and mechanistic study. J Environ Manag 258:110032

    Article  CAS  Google Scholar 

  • Hammouda SB, Fourcade F, Assadi A, Soutrel I, Amrane A, Monser L (2016) Effective heterogeneous electro-Fenton process for the degradation of a malodorous compound, indole, using iron loaded alginate beads as a reusable catalyst. Appl Catal B Environ 182:47–58

    Article  Google Scholar 

  • Hiwarkar AD, Singh S, Srivastava VC, Thakur C, Mall ID, Lo SL (2018) Electrochemical mineralization of recalcitrant indole by platinum-coated titanium electrode: multi-response optimization, mechanistic and sludge disposal study. Int J Environ Sci Technol 15:349–360

    Article  CAS  Google Scholar 

  • Jeyasubramanian K, Hikku GS, Sharma RK (2015) Photo-catalytic degradation of methyl violet dye using zinc oxide nano particles prepared by a novel precipitation method and its anti-bacterial activities. J Water Process Eng 8:35–44

    Article  Google Scholar 

  • Jiang N, Zhao Q, Xue Y, Xu W, Ye Z (2018) Removal of dinitrotoluene sulfonate from explosive wastewater by electrochemical method using Ti/IrO2 as electrode. J Clean Prod 188:732–740

    Article  CAS  Google Scholar 

  • Kumar S, Singh S, Srivastava VC (2015) Electro-oxidation of nitrophenol by ruthenium oxide coated titanium electrode: parametric, kinetic and mechanistic study. Chem Eng J 263:135–143

    Article  CAS  Google Scholar 

  • Kushwaha JP, Srivastava VC, Mall ID (2011) Studies on electrochemical treatment of dairy wastewater using aluminum electrode. AICHE J 57(9):2589–2598

    Article  CAS  Google Scholar 

  • Li M, Gao X, Liu H, Wang H, Zhao Q, Wang N (2020) Preparation of heterogeneous Fenton catalyst γ-Cu-Ce-Al2O3 and the evaluation on degradation of phenol. Environ Sci Pollut Res 1-11

  • Mahajan BK, Kumar N, Chauhan R, Srivastava VC, Gulati S (2019) Mechanistic evaluation of heterocyclic aromatic compounds mineralization by a Cu doped ZnO photo-catalyst. Photochem Photobiol Sci 18:1540–1555

    Article  CAS  Google Scholar 

  • Mahesh S, Prasad B, Mall ID, Mishra IM (2006) Electrochemical degradation of pulp and paper mill wastewater. Part 1. COD and color removal. Ind Eng Chem Res 45:2830–2839

    Article  CAS  Google Scholar 

  • Martínez-Huitle CA, Ferro S (2006) Electrochemical oxidation of organic pollutants for the wastewater treatment: direct and indirect processes. Chem Soc Rev 35:1324–1340

    Article  Google Scholar 

  • McCombs NL, Smirnova T, Ghiladi RA (2017) Oxidation of pyrrole by dehaloperoxidase-hemoglobin: chemoenzymatic synthesis of pyrrolin-2-ones. Catal Sci Technol 7:3104–3118

    Article  CAS  Google Scholar 

  • Mondal B, Srivastava VC, Kushwaha JP, Bhatnagar R, Singh S, Mall ID (2013) Parametric and multiple response optimization for the electrochemical treatment of textile printing dye-bath effluent. Sep Purif Technol 109:135–143

    Article  CAS  Google Scholar 

  • Novotny M, Strand JW, Smith SL, Wiesler D, Schwende FJ (1981) Compositional studies of coal tar by capillary gas chromatography mass spectrometry. Fuel 60(3):213–220

    Article  CAS  Google Scholar 

  • Padoley KV, Mudliar SN, Banerjee SK, Deshmukh SC, Pandey RA (2011) Fenton oxidation: a pretreatment option for improved biological treatment of pyridine and 3-cyanopyridine plant wastewater. Chem Eng J 166:1–9

    Article  CAS  Google Scholar 

  • Panizza M, Cerisola G (2009) Direct and mediated anodic oxidation of organic pollutants. Chem Rev 109:6541–6569

    Article  CAS  Google Scholar 

  • Paudler WW, Cheplen M (1979) Nitrogen bases in solvent-refined coal. Fuel 58:775–778

    Article  CAS  Google Scholar 

  • Sandhwar VK, Prasad B (2019) A comparative study of electrochemical degradation of benzoic acid and terephthalic acid from aqueous solution of purified terephthalic acid (PTA) wastewater. J Water Process Eng 30:100381

    Article  Google Scholar 

  • Sharma P, Kumar N, Chauhan R, Singh V, Srivastava VC, Bhatnagar R (2020) Growth of hierarchical ZnO nano flower on large functionalized rGO sheet for superior photocatalytic mineralization of antibiotic. Chem Eng J 392:123746

    Article  CAS  Google Scholar 

  • Singh V, Srivastava VC (2020) Self-engineered iron oxide nanoparticle incorporated on mesoporous biochar derived from textile mill sludge for the removal of an emerging pharmaceutical pollutant. Environ Pollut 259:113822

    Article  CAS  Google Scholar 

  • Singh S, Lo SL, Srivastava VC, Hiwarkar AD (2016) Comparative study of electrochemical oxidation for dye degradation: parametric optimization and mechanism identification. J Environ Chem Eng 4:2911–2921

    Article  CAS  Google Scholar 

  • Srivastava VC, Mall ID, Mishra IM (2007) Multicomponent adsorption study of metal ions onto bagasse fly ash using Taguchi’s design of experimental methodology. Ind Eng Chem Res 46:5697–5706

    Article  CAS  Google Scholar 

  • Subbaramaiah V, Srivastava VC, Mall ID (2013a) Catalytic wet peroxidation of pyridine bearing wastewater by cerium supported SBA-15. J Hazard Mater 248–249:355–363

    Article  Google Scholar 

  • Subbaramaiah V, Srivastava VC, Mall ID (2013b) Catalytic activity of Cu/SBA-15 for peroxidation of pyridine bearing wastewater at atmospheric condition. AIChE J 59(7):2577–2586

  • Xing X, Zhu X, Li H, Jiang Y, Ni J (2012) Electrochemical oxidation of nitrogen-heterocyclic compounds at boron-doped diamond electrode. Chemosphere 86:368–375

    Article  CAS  Google Scholar 

  • Xue L, Liu J, Li M, Tan L, Ji X, Shi S, Jiang B (2017) Enhanced treatment of coking wastewater containing phenol, pyridine, and quinoline by integration of an E-Fenton process into biological treatment. Environ Sci Pollut Res 24:9765–9775

    Article  CAS  Google Scholar 

  • Yousefieh M, Shamanian M, Saatchi A (2012) Optimization of experimental conditions of the pulsed current GTAW parameters for mechanical properties of SDSS UNS S32760 welds based on the Taguchi design method. J Mater Eng Perform 21:1978–1988

    Article  CAS  Google Scholar 

  • Zhou X, Liu S, Yu H, Xu A, Li J, Sun X, Shen J, Han W, Wang L (2018) Electrochemical oxidation of pyrrole, pyrazole and tetrazole using a TiO2 nanotubes based SnO2-Sb/3D highly ordered macro-porous PbO2 electrode. J Electroanal Chem 826:181–190

    Article  CAS  Google Scholar 

  • Zhu H, Ma W, Han H, Xu C, Han Y, Ma W (2018) Degradation characteristics of two typical N-heterocycles in ozone process: efficacy, kinetics, pathways, toxicity and its application to real biologically pretreated coal gasification wastewater. Chemosphere 209:319–327

    Article  CAS  Google Scholar 

  • Zingler E (1969) Significance and limits of Buchner funnel filtration test. In Proc. 5th Int. Conf. Wat Pollut res (Vol. 1)

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Acknowledgements

Authors thank Quality Improvement Programme (QIP) of All India Council for Technical Education (AICTE), India, and Ministry of Human Resources and Development (MHRD), India, for providing their financial support.

Funding

Quality Improvement Programme (QIP) of All India Council for Technical Education (AICTE), India; and Ministry of Human Resources and Development (MHRD), India.

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Authors and Affiliations

  1. Department of Chemical Engineering, Indian Institute of Technology, Roorkee, Roorkee, Uttarakhand, 247667, India

    Ajay Devidas Hiwarkar, Rohit Chauhan, Ritesh Patidar, Vimal Chandra Srivastava, Seema Singh & Indra Deo Mall

  2. Department of Chemical Engineering, Bundelkhand Institute of Engineering and Technology, Jhansi, Uttar Pradesh, 284128, India

    Ajay Devidas Hiwarkar

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  1. Ajay Devidas Hiwarkar
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  2. Rohit Chauhan
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  4. Vimal Chandra Srivastava
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  5. Seema Singh
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  6. Indra Deo Mall
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Contributions

Material preparation, data collection and analysis were performed by Ajay Devidas Hiwarkar (ADH), Rohit Chauhan (RC), Ritesh Patidar (RP) and Seema Singh (SS). The first draft of the manuscript was written by Rohit Chauhan (RC) and Ritesh Patidar (RP) and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

Conceptualization: Vimal Chandra Srivastava (VCS) and Indra Deo Mall (IDM); Methodology: Vimal Chandra Srivastava (VCS), Indra Deo Mall (IDM), Ajay Devidas Hiwarkar (ADH) and Seema Singh (SS).

Formal analysis and investigation: Ajay Devidas Hiwarkar (ADH), Rohit Chauhan (RC) and Ritesh Patidar (RP)

Writing - original draft preparation: Ajay Devidas Hiwarkar (ADH), Rohit Chauhan (RC)] and Ritesh Patidar (RP);

Writing - review and editing: Rohit Chauhan (RC) and Ritesh Patidar (RP);

Funding acquisition: Ajay Devidas Hiwarkar (ADH);

Software: Ajay Devidas Hiwarkar (ADH) and Ritesh Patidar (RP)

Supervision: Vimal Chandra Srivastava (VCS) and Indra Deo Mall (IDM).

Corresponding author

Correspondence to Vimal Chandra Srivastava.

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Hiwarkar, A.D., Chauhan, R., Patidar, R. et al. Binary electrochemical mineralization of heterocyclic nitrogenous compounds: parametric optimization using Taguchi method and mineralization mechanism. Environ Sci Pollut Res 28, 7332–7346 (2021). https://doi.org/10.1007/s11356-020-11057-8

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