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Modification of graphite felt doped with nitrogen and boron for enhanced removal of dimethyl phthalate in peroxi-coagulation system and mechanisms

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Abstract

To enhance the generation of hydrogen peroxide (H2O2), a modified graphite felt cathode doped with nitrogen and boron was developed and used in peroxi-coagulation system to degrade dimethyl phthalate (DMP). After a simple modification method, the yield of H2O2 on cathode increased from 9.39 to 152.8 mg/L, with current efficiency increased from 1.61 to 70.3%. Complete degradation of DMP and 80% removal of TOC were achieved within 2 h at the optimal condition with pH of 5, cathodic potential of − 0.69 V (vs. SCE), oxygen aeration, and electrode gap of 1 cm. Possible mechanism with synergistic effect of electro-Fenton and electrocoagulation process in the peroxi-coagulation system was revealed via quenching experiments. The prospect of this system in the effluent of landfill leachate and domestic sewage was studied, achieving 50% and 61% of DMP removal in 2 h. This efficient system with simple modified cathode had promising prospects in practical applications.

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References

  • Agnoli S, Favaro M (2016) Doping graphene with boron: a review of synthesis methods, physicochemical characterization, and emerging applications. J Mater Chem A 4:5002–5025

    CAS  Google Scholar 

  • Asghar A, Raman AAA, Daud WMAW, Ramalingam A, Zain SBM (2019) Determining the feasibility of H2O2 production at a graphite cathode using bond dissociation energy: comparing simple and nitrogen doped cathodes. Res Chem Intermed 45:3311–3327

    CAS  Google Scholar 

  • Barrera-Diaz C, Canizares P, Fernandez FJ, Natividad R, Rodrigo MA (2014) Electrochemical advanced oxidation processes: an overview of the current applications to actual industrial effluents. J Mex Chem Soc 58:256–275

    CAS  Google Scholar 

  • Bolton JR, Bircher KG, Tumas W, Tolman CA (2001) Figures-of-merit for the technical development and application of advanced oxidation technologies for both electric- and solar-driven systems - (IUPAC technical report). Pure Appl Chem 73:627–637

    CAS  Google Scholar 

  • Brillas E, Garcia-Segura S (2020) Benchmarking recent advances and innovative technology approaches of Fenton, photo-Fenton, electro-Fenton, and related processes: a review on the relevance of phenol as model molecule. Sep Purif Technol 237:116337

    Google Scholar 

  • Brillas E, Sires I, Oturan MA (2009) Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry. Chem Rev 109:6570–6631

    CAS  Google Scholar 

  • Casado J (2019) Towards industrial implementation of Electro-Fenton and derived technologies for wastewater treatment: a review. J Environ Chem Eng 7:102823

    CAS  Google Scholar 

  • Chang Y, Yuan C, Li Y, Liu C, Wu T, Zeng B, Xu Y, Dai L (2017) Controllable fabrication of a N and B co-doped carbon shell on the surface of TiO2 as a support for boosting the electrochemical performances. J Mater Chem A 5:1672–1678

    CAS  Google Scholar 

  • Chaplin BP (2014) Critical review of electrochemical advanced oxidation processes for water treatment applications. Environ Sci-Proc Imp 16:1182–1203

    CAS  Google Scholar 

  • Chen W, Lin S (2009) Destruction of nitrotoluenes in wastewater by electro-Fenton oxidation. J Hazard Mater 168:1562–1568

    CAS  Google Scholar 

  • Chu Y, Zhang D, Liu L, Qian Y, Li L (2013) Electrochemical degradation of m-cresol using porous carbon-nanotube-containing cathode and Ti/SnO2-Sb2O5-IrO2 anode: kinetics, byproducts and biodegradability. J Hazard Mater 252:306–312

    Google Scholar 

  • Colades JI, Huang CP, Retumban JD, Garcia-Segura S, de Luna MDG (2020) Electrochemically-driven dosing of iron (II) for autonomous electro-Fenton processes with in situ generation of H2O2. J Electroanal Chem 856:113639

    CAS  Google Scholar 

  • Deng Y, Englehardt JD (2006) Treatment of landfill leachate by the Fenton process. Water Res 40:3683–3694

    CAS  Google Scholar 

  • Ding W, Li L, Xiong K, Wang Y, Li W, Nie Y, Chen S, Qi X, Wei Z (2015) Shape fixing via salt recrystallization: a morphology-controlled approach to convert nanostructured polymer to carbon nanomaterial as a highly active catalyst for oxygen reduction reaction. J Am Chem Soc 137:5414–5420

    CAS  Google Scholar 

  • Garcia-Segura S, Brillas E (2017) Applied photoelectrocatalysis on the degradation of organic pollutants in wastewaters. J Photochem Photobiol C 31:1–35

    CAS  Google Scholar 

  • Garcia-Segura S, Salazar R, Brillas E (2013) Mineralization of phthalic acid by solar photoelectro-Fenton with a stirred boron-doped diamond/air-diffusion tank reactor: influence of Fe3+ and Cu2+ catalysts and identification of oxidation products. Electrochim Acta 113:609–619

    CAS  Google Scholar 

  • Garcia-Segura S, Eiband MMSG, de Melo JV, Martinez-Huitle CA (2017) Electrocoagulation and advanced electrocoagulation processes: a general review about the fundamentals, emerging applications and its association with other technologies. J Electroanal Chem 801:267–299

    CAS  Google Scholar 

  • Jiang Z, Zhao X, Tian X, Luo L, Fang J, Gao H, Jiang Z (2015) Hydrothermal synthesis of boron and nitrogen codoped hollow graphene microspheres with enhanced electrocatalytic activity for oxygen reduction reaction. ACS Appl Mater Interfaces 7:19398–19407

    CAS  Google Scholar 

  • Kamaraj R, Vasudevan S (2019) Sulfur-doped carbon chain network as high-performance Electrocatalyst for electro-Fenton system. Chemistryselect 4:2428–2435

    CAS  Google Scholar 

  • Kim SM, Vogelpohl A (1998) Degradation of organic pollutants by the photo-Fenton-process. Chem Eng Technol 21:187–191

    CAS  Google Scholar 

  • Lanzarini-Lopes M, Garcia-Segura S, Hristovski K, Westerhoff P (2017) Electrical energy per order and current efficiency for electrochemical oxidation of p-chlorobenzoic acid with boron-doped diamond anode. Chemosphere 188:304–311

    CAS  Google Scholar 

  • Lei H, Li H, Li Z, Li Z, Chen K, Zhang X, Wang H (2010) Electro-Fenton degradation of cationic red X-GRL using an activated carbon fiber cathode. Process Saf Environ 88:431–438

    CAS  Google Scholar 

  • Li C, Huang Y, Dong X, Sun Z, Duan X, Ren B, Zheng S, Dionysiou DD (2019) Highly efficient activation of peroxymonosulfate by natural negatively-charged kaolinite with abundant hydroxyl groups for the degradation of atrazine. Appl Catal B Environ 247:10–23

    CAS  Google Scholar 

  • Liu T, Wang K, Song S, Brouzgou A, Tsiakaras P, Wang Y (2016) New electro-Fenton gas diffusion cathode based on nitrogen-doped Graphene@carbon nanotube composite materials. Electrochim Acta 194:228–238

    CAS  Google Scholar 

  • Liu X, Yang D, Zhou Y, Zhang J, Luo L, Meng S, Chen S, Tan M, Li Z, Tang L (2017) Electrocatalytic properties of N-doped graphite felt in electro-Fenton process and degradation mechanism of levofloxacin. Chemosphere 182:306–315

    CAS  Google Scholar 

  • Liu Y, Feng Y, Zhang Y, Mao S, Wu D, Chu H (2019) Highly efficient degradation of dimethyl phthalate from cu(II) and dimethyl phthalate wastewater by EDTA enhanced ozonation: performance, intermediates and mechanism. J Hazard Mater 366:378–385

    CAS  Google Scholar 

  • Molina-Garcia MA, Rees NV (2018) "metal-free" electrocatalysis: quaternary-doped graphene and the alkaline oxygen reduction reaction. Appl Catal A Gen 553:107–116

    CAS  Google Scholar 

  • Moore NP (2000) The oestrogenic potential of the phthalate esters. Reprod Toxicol 14:183–192

    CAS  Google Scholar 

  • Moreira FC, Boaventura RAR, Brillas E, Vilar VJP (2017) Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Appl Catal B Environ 202:217–261

    CAS  Google Scholar 

  • Moreira J, Lima VB, Goulart LA, Lanza MRV (2019) Electrosynthesis of hydrogen peroxide using modified gas diffusion electrodes (MGDE) for environmental applications: quinones and azo compounds employed as redox modifiers. Appl Catal B Environ 248:95–107

    CAS  Google Scholar 

  • Puziy AM, Poddubnaya OI, Martinez-Alonso A, Suarez-Garcia F, Tascon J (2002) Synthetic carbons activated with phosphoric acid - II. Porous structure. Carbon 40:1507–1519

    CAS  Google Scholar 

  • Qiu S, Yu L, Tang D, Ren W, Chen K, Sun J (2018) Rapidly enhanced electro-Fenton efficiency by in situ electrochemistry-activated graphite cathode. Ind Eng Chem Res 57:4907–4915

    CAS  Google Scholar 

  • Ren W, Peng Q, Huang Z, Zhang Z, Zhan W, Lv K, Sun J (2015) Effect of pore structure on the electro-Fenton activity of ACF@OMC cathode. Ind Eng Chem Res 54:8492–8499

    CAS  Google Scholar 

  • Ren G, Zhou M, Su P, Liang L, Yang W, Mousset E (2018) Highly energy-efficient removal of acrylonitrile by peroxi-coagulation with modified graphite felt cathode: influence factors, possible mechanism. Chem Eng J 343:467–476

    CAS  Google Scholar 

  • Rodrigo MA, Oturan N, Oturan MA (2014) Electrochemically assisted remediation of pesticides in soils and water: a review. Chem Rev 114:8720–8745

    CAS  Google Scholar 

  • Sellers RM (1980) Spectrophotometric determination of hydrogen peroxide using potassium titanium(IV) oxalate. Analyst 105:950–954

    CAS  Google Scholar 

  • Shandilya P, Mittal D, Soni M, Raizada P, Hosseini-Bandegharaei A, Saini AK, Singh P (2018) Fabrication of fluorine doped graphene and SmVO4 based dispersed and adsorptive photocatalyst for abatement of phenolic compounds from water and bacterial disinfection. J Clean Prod 203:386–399

    CAS  Google Scholar 

  • Sheng Z, Shao L, Chen J, Bao W, Wang F, Xia X (2011) Catalyst-free synthesis of nitrogen-doped graphene via thermal annealing graphite oxide with melamine and its excellent electrocatalysis. ACS Nano 5:4350–4358

    CAS  Google Scholar 

  • Sheng Z, Gao H, Bao W, Wang F, Xia X (2012) Synthesis of boron doped graphene for oxygen reduction reaction in fuel cells. J Mater Chem 22:390–395

    CAS  Google Scholar 

  • Wang T, Liu T (2017) Pulse electro-coagulation application in treating dibutyl phthalate wastewater. Water Sci Technol 76:1124–1131

    CAS  Google Scholar 

  • Wang S, Iyyamperumal E, Roy A, Xue Y, Yu D, Dai L (2011) Vertically aligned BCN nanotubes as efficient metal-free electrocatalysts for the oxygen reduction reaction: a synergetic effect by co-doping with boron and nitrogen. Angew Chem Int Ed 50:11756–11760

    CAS  Google Scholar 

  • Wang Y, Liu Y, Liu T, Song S, Gui X, Liu H, Tsiakaras P (2014) Dimethyl phthalate degradation at novel and efficient electro-Fenton cathode. Appl Catal B Environ 156:1–7

    Google Scholar 

  • Wang D, Duan X, He X, Dionysiou DD (2016a) Degradation of dibutyl phthalate (DBP) by UV-254 nm/H2O2 photochemical oxidation: kinetics and influence of various process parameters. Environ Sci Pollut Res 23:23772–23780

  • Wang Y, Ao Z, Sun H, Duan X, Wang S (2016b) Activation of peroxymonosulfate by carbonaceous oxygen groups: experimental and density functional theory calculations. Appl Catal B Environ 198:295–302

  • Wang T, Qu G, Yin X, Sun Q, Liang D, Guo X, Jia H (2018) Dimethyl phthalate elimination from micro-polluted source water by surface discharge plasma: performance, active species roles and mechanisms. J Hazard Mater 357:279–288

    CAS  Google Scholar 

  • Wang Y, Zhou W, Gao J, Ding Y, Kou K (2019) Oxidative modification of graphite felts for efficient H2O2 electrogeneration: enhancement mechanism and long-term stability. J Electroanal Chem 833:258–268

    CAS  Google Scholar 

  • Wu J, Jin C, Yang Z, Tian J, Yang R (2015) Synthesis of phosphorus-doped carbon hollow spheres as efficient metal-free electrocatalysts for oxygen reduction. Carbon 82:562–571

    CAS  Google Scholar 

  • Xu TL, Kamat PV, O'Shea KE (2005) Mechanistic evaluation of arsenite oxidation in TiO2 assisted photocatalysis. J Phys Chem A 109:9070–9075

    CAS  Google Scholar 

  • Yao Y, Chen H, Qin J, Wu G, Lian C, Zhang J, Wang S (2016) Iron encapsulated in boron and nitrogen codoped carbon nanotubes as synergistic catalysts for Fenton-like reaction. Water Res 101:281–291

    CAS  Google Scholar 

  • Yu F, Zhou M, Yu X (2015) Cost-effective electro-Fenton using modified graphite felt that dramatically enhanced on H2O2 electro-generation without external aeration. Electrochim Acta 163:182–189

    CAS  Google Scholar 

  • Yu J, Liu T, Liu H, Wang Y (2016) Electro-polymerization fabrication of PANI@GF electrode and its energy-effective electrocatalytic performance in electro-Fenton process. Chin J Catal 37:2079–2085

    CAS  Google Scholar 

  • Zhang J, Zhou W, Yang L, Chen Y, Hu Y (2018) Co-N-doped MoO2 modified carbon felt cathode for removal of EDTA-Ni in electro-Fenton process. Environ Sci Pollut Res 25:22754–22765

    CAS  Google Scholar 

  • Zhang D, Liu T, Yin K, Liu C, Wei Y (2020) Selective H2O2 production on N-doped porous carbon from direct carbonization of metal organic frameworks for electro-Fenton mineralization of antibiotics. Chem Eng J 383:123184

    Google Scholar 

  • Zhao L, He R, Rim KT, Schiros T, Kim KS, Zhou H, Gutierrez C, Chockalingam SP, Arguello CJ, Palova L, Nordlund D, Hybertsen MS, Reichman DR, Heinz TF, Kim P, Pinczuk A, Flynn GW, Pasupathy AN (2011) Visualizing individual nitrogen dopants in monolayer graphene. Science 333:999–1003

    CAS  Google Scholar 

  • Zheng Y, Jiao Y, Ge L, Jaroniec M, Qiao SZ (2013) Two-step boron and nitrogen doping in graphene for enhanced synergistic catalysis. Angew Chem Int Ed 52:3110–3116

    CAS  Google Scholar 

  • Zheng W, Xiao X, Chen B (2019) A nonradical reaction-dominated phenol degradation with peroxydisulfate catalyzed by nitrogen-doped graphene. Sci Total Environ 667:287–296

    CAS  Google Scholar 

  • Zhou L, Hu Z, Zhang C, Bi Z, Jin T, Zhou M (2013) Electrogeneration of hydrogen peroxide for electro-Fenton system by oxygen reduction using chemically modified graphite felt cathode. Sep Purif Technol 111:131–136

    CAS  Google Scholar 

  • Zhou L, Zhou M, Hu Z, Bi Z, Serrano KG (2014) Chemically modified graphite felt as an efficient cathode in electro-Fenton for p-nitrophenol degradation. Electrochim Acta 140:376–383

    CAS  Google Scholar 

  • Zhou Y, Sun Y, Wang H, Zhu C, Gao J, Wu D, Huang H, Liu Y, Kang Z (2018) A nitrogen and boron co-doped metal-free carbon electrocatalyst for an efficient oxygen reduction reaction. Inorg Chem Front 5:2985–2991

    CAS  Google Scholar 

Download references

Acknowledgments

The authors acknowledged the support from Open Project of State Key Laboratory of Urban Water Resource and Environment (QA201926), China Postdoctoral Science Foundation funded projects (2017M611373), Fundamental Research Funds for the Central Universities (HIT. NSRIF. 201858), and the Nature Science Foundation of Heilongjiang (E2017047).

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Authors and Affiliations

  1. State Key Laboratory of Urban Water Resources and Environment (SKLUWRE), School of Environment, Harbin Institute of Technology, Harbin, 150090, China

    Jing Ding, Langang Dong, Yuxuan Geng, Huibin Huang, Guanshu Zhao, Junqiu Jiang, Shan Qiu, Yixing Yuan & Qingliang Zhao

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  1. Jing Ding
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  2. Langang Dong
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  3. Yuxuan Geng
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  4. Huibin Huang
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  7. Shan Qiu
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  8. Yixing Yuan
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  9. Qingliang Zhao
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Correspondence to Qingliang Zhao.

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Ding, J., Dong, L., Geng, Y. et al. Modification of graphite felt doped with nitrogen and boron for enhanced removal of dimethyl phthalate in peroxi-coagulation system and mechanisms. Environ Sci Pollut Res 27, 18810–18821 (2020). https://doi.org/10.1007/s11356-020-08384-1

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