Advertisement

Environmental Science and Pollution Research

, Volume 22, Issue 20, pp 15812–15820 | Cite as

Enhanced hydroxyl radical generation in the combined ozonation and electrolysis process using carbon nanotubes containing gas diffusion cathode

  • Donghai Wu
  • Guanghua LuEmail author
  • Ran Zhang
  • Qiuhong Lin
  • Zhenhua Yan
  • Jianchao Liu
  • Yi Li
Research Article

Abstract

Combination of ozone together with electrolysis (ozone-electrolysis) is a promising wastewater treatment technology. This work investigated the potential use of carbon nanotube (CNT)-based gas diffusion cathode (GDC) for ozone-electrolysis process employing hydroxyl radicals (·OH) production as an indicator. Compared with conventional active carbon (AC)-polytetrafluoroethylene (PTFE) and carbon black (CB)-PTFE cathodes, the production of ·OH in the coupled process was improved using CNTs-PTFE GDC. Appropriate addition of acetylene black (AB) and pore-forming agent Na2SO4 could enhance the efficiency of CNTs-PTFE GDC. The optimum GDC composition was obtained by response surface methodology (RSM) analysis and was determined as CNTs 31.2 wt%, PTFE 60.6 wt%, AB 3.5 wt%, and Na2SO4 4.7 wt%. Moreover, the optimized CNT-based GDC exhibited much more effective than traditional Ti and graphite cathodes in Acid Orange 7 (AO7) mineralization and possessed the desirable stability without performance decay after ten times reaction. The comparison tests revealed that peroxone reaction was the main pathway of ·OH production in the present system, and cathodic reduction of ozone could significantly promote ·OH generation. These results suggested that application of CNT-based GDC offers considerable advantages in ozone-electrolysis of organic wastewater.

Keywords

Ozone-electrolysis Gas diffusion cathode Carbon nanotubes Hydroxyl radicals Response surface methodology 

Nomenclature

AB

Acetylene black

AC

Active carbon

AOPs

Advanced oxidation processes

AO7

Acid Orange 7

ANOVA

Analysis of variances

BBD

Box-Behnken design

CB

Carbon black

CNTs

Carbon nanotubes

C.V.

Coefficient of variation

DDI

Deionized-distilled

GDC

Gas diffusion cathode

O3

Ozone

·OH

Hydroxyl radicals

pCBA

p-Chlorobenzoic acid

PTFE

Polytetrafluoroethylene

R2

Coefficient of determination

RSM

Response surface methodology

SEM

Scanning electron microscopy

TOC

Total organic carbon

Notes

Acknowledgments

We are grateful for grants from Natural Science Foundation of Jiangsu Province (No. BK20130835), China Postdoctoral Science Foundation (No. 2013 M541600), Fundamental Research Funds for the Central Universities of Hohai University (No. 2013B13020026), and A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Supplementary material

11356_2015_4783_MOESM1_ESM.doc (74 kb)
ESM 1 (DOC 74 kb)

References

  1. APHA (1998) Standard Methods for the Examination of Water and Wastewater, 20th edn. American Public Health Association Washington DC, USAGoogle Scholar
  2. Bakheet B, Yuan S, Li Z, Wang H, Zuo J, Komarneni S, Wang Y (2013) Electro-peroxone treatment of Orange II dye wastewater. Water Res 47:6234–6243CrossRefGoogle Scholar
  3. Bakheet B, Qiu C, Yuan S, Wang Y, Yu G, Deng S, Huang J, Wang B (2014) Inhibition of polymer formation in electrochemical degradation of p-nitrophenol by combining electrolysis with ozonation. Chem Eng J 252:17–21CrossRefGoogle Scholar
  4. Barros WRP, Reis RM, Rocha RS, Lanza MRV (2013) Electrogeneration of hydrogen peroxide in acidic medium using gas diffusion electrodes modified with cobalt (II) phthalocyanine. Electrochim Acta 104:12–18CrossRefGoogle Scholar
  5. Beltrán FJ, Ovejero G, Rivas J (1996) Oxidation of polynuclear aromatic hydrocarbons in water.4. Ozone combined with hydrogen peroxide. Ind Eng Chem Res 35:891–898CrossRefGoogle Scholar
  6. Brillas E, Sires I, Oturan MA (2009) Electro-fenton process and related electrochemical technologies based on fenton’s reaction chemistry. Chem Rev 109:6570–6631CrossRefGoogle Scholar
  7. Chang J, Chen ZL, Wang Z, Shen JM, Chen Q, Kang J, Yang L, Liu XW, Nie CX (2014) Ozonation degradation of microcystin-LR in aqueous solution: intermediates, byproducts and pathways. Water Res 63:52–61CrossRefGoogle Scholar
  8. Cho M, Chung H, Choi W, Yoon J (2004) Linear correlation between inactivation of E. coli and OH radical concentration in TiO2 photocatalytic disinfection. Water Res 38:1069–1077CrossRefGoogle Scholar
  9. Fan XL, Restivo J, Orfao JJM, Pereira MFR, Lapkin AA (2014) The role of multiwalled carbon nanotubes (MWCNTs) in the catalytic ozonation of atrazine. Chem Eng J 241:66–76CrossRefGoogle Scholar
  10. García-Gómez C, Drogui P, Zaviska F, Seyhi B, Gortáres-Moroyoqui P, Buelna G, Neira-Sáenz C, Estrada-alvarado M, Ulloa-Mercado RG (2014) Experimental design methodology applied to electrochemical oxidation of carbamazepine using Ti/PbO2 and Ti/BDD electrodes. J Electroanal Chem 732:1–10CrossRefGoogle Scholar
  11. Garcia-Morales MA, Roa-Morales G, Barrera-Diaz C, Bilyeu B, Rodrigo MA (2013) Synergy of electrochemical oxidation using boron-doped diamond (BDD) electrodes and ozone (O3) in industrial wastewater treatment. Electrochem Commun 27:34–37CrossRefGoogle Scholar
  12. Gedam N, Neti NR, Kashyap SM (2014) Treatment of recalcitrant caprolactam wastewater using electrooxidation and ozonation. Clean-Soil Air Water 42:932–938CrossRefGoogle Scholar
  13. Giorgi L, Antolini E, Pozio A, Passalacqua E (1998) Influence of the PTFE content in the diffusion layer of low-Pt loading electrodes for polymer electrolyte fuel cells. Electrochim Acta 43:3675–3680CrossRefGoogle Scholar
  14. Hermosilla D, Merayo N, Gasco A, Blanco A (2015) The application of advanced oxidation technologies to the treatment of effluents from the pulp and paper industry: a review. Environ Sci Pollut Res Int 22:168–191CrossRefGoogle Scholar
  15. Hsu YC, Chen YF, Chen JH (2003) Peroxone process for RO-16 and RB-19 dye solutions treatment. J Environ Sci Heal A 38:1361–1376CrossRefGoogle Scholar
  16. Huang H, Zhang W, Li M, Gan Y, Chen J, Kuang Y (2005) Carbon nanotubes as a secondary support of a catalyst layer in a gas diffusion electrode for metal air batteries. J Colloid Interface Sci 284:593–599CrossRefGoogle Scholar
  17. Khataee AR, Safarpour M, Zarei M, Aber S (2011) Electrochemical generation of H2O2 using immobilized carbon nanotubes on graphite electrode fed with air: Investigation of operational parameters. J Electroanal Chem 659:63–68CrossRefGoogle Scholar
  18. Khataee A, Safarpour M, Vahid B, Akbarpour A (2014) Degrading a mixture of three textile dyes using photo-assisted electrochemical process with BDD anode and O2-diffusion cathode. Environ Sci Pollut Res 21:8543–8554CrossRefGoogle Scholar
  19. Kishimoto N, Morita Y, Tsuno H, Oomura T, Mizutani H (2005) Advanced oxidation effect of ozonation combined with electrolysis. Water Res 39:4661–4672CrossRefGoogle Scholar
  20. Kishimoto N, Nakagawa T, Asano M, Abe M, Yamada M, Ono Y (2008) Ozonation combined with electrolysis of 1,4-dioxane using a two-compartment electrolytic flow cell with solid electrolyte. Water Res 42:379–385CrossRefGoogle Scholar
  21. Li Z, Yuan S, Qiu C, Wang Y, Pan X, Wang J, Wang C, Zuo J (2013) Effective degradation of refractory organic pollutants in landfill leachate by electro-peroxone treatment. Electrochim Acta 102:174–182CrossRefGoogle Scholar
  22. Li X, Wang Y, Yuan S, Li Z, Wang B, Huang J, Deng S, Yu G (2014) Degradation of the anti-inflammatory drug ibuprofen by electro-peroxone process. Water Res 63:81–93CrossRefGoogle Scholar
  23. Li Y, Shen W, Fu S, Yang H, Yu G, Wang Y (2015) Inhibition of bromate formation during drinking water treatment by adapting ozonation to electro-peroxone process. Chem Eng J 264:322–328CrossRefGoogle Scholar
  24. Maja M, Orecchia C, Strano M, Tosco P, Vanni M (2000) Effect of structure of the electrical performance of gas diffusion electrodes for metal air batteries. Electrochim Acta 46:423–432CrossRefGoogle Scholar
  25. Neta P, Dorfman LM (1968) Pulse radiolysis studies, XIII: rate constants for the reaction of hydroxyl radicals with aromatic compounds in aqueous solutions. Adv Chem Ser 81:222–230CrossRefGoogle Scholar
  26. Oturan N, Wu J, Zhang H, Sharma VK, Oturan MA (2013) Electrocatalytic destruction of the antibiotic tetracycline in aqueous medium by electrochemical advanced oxidation processes: Effect of electrode materials. Appl Catal B-Environ 140:92–97CrossRefGoogle Scholar
  27. Parsa JB, Golmirzaei M, Abbasi M (2014) Degradation of azo dye C.I. Acid Red 18 in aqueous solution by ozone-electrolysis process. J Ind Eng Chem 20:689–694CrossRefGoogle Scholar
  28. Qiu C, Yuan S, Li X, Wang H, Bakheet B, Komarneni S, Wang Y (2014) Investigation of the synergistic effects for p-nitrophenol mineralization by a combined process of ozonation and electrolysis using a boron-doped diamond anode. J Hazard Mater 280:644–653CrossRefGoogle Scholar
  29. Soltani RDC, Rezaee A, Khataee AR, Godini H (2012) Electrochemical generation of hydrogen peroxide using carbon black-, carbon nanotube-, and carbon black/carbon nanotube-coated gas-diffusion cathodes: effect of operational parameters and decolorization study. Res Chem Intermed 39:4277–4286CrossRefGoogle Scholar
  30. Vahid B, Khataee A (2013) Photoassisted electrochemical recirculation system with boron-doped diamond anode and carbon nanotubes containing cathode for degradation of a model azo dye. Electrochim Acta 88:614–620CrossRefGoogle Scholar
  31. Vijayalakshmi P, Raju GB, Gnanamani A (2011) Advanced Oxidation and Electrooxidation As Tertiary Treatment Techniques to Improve the Purity of Tannery Wastewater. Ind Eng Chem Res 50:10194–10200CrossRefGoogle Scholar
  32. Wang Y, Li X, Zhen L, Zhang H, Zhang Y, Wang C (2012) Electro-Fenton treatment of concentrates generated in nanofiltration of biologically pretreated landfill leachate. J Hazard Mater 229–230:115–121CrossRefGoogle Scholar
  33. Xu WY, Li P, Dong B (2010) Electrochemical disinfection using the gas diffusion electrode system. J Environ Sci-China 22:204–210CrossRefGoogle Scholar
  34. Yuan S, Li ZX, Wang YJ (2013) Effective degradation of methylene blue by a novel electrochemically driven process. Electrochem Commun 29:48–51CrossRefGoogle Scholar
  35. Zhang Z-y, Xu X-c (2014) Wrapping carbon nanotubes with poly (sodium 4-styrenesulfonate) for enhanced adsorption of methylene blue and its mechanism. Chem Eng J 256:85–92CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  • Donghai Wu
    • 1
  • Guanghua Lu
    • 1
    Email author
  • Ran Zhang
    • 2
  • Qiuhong Lin
    • 1
  • Zhenhua Yan
    • 1
  • Jianchao Liu
    • 1
  • Yi Li
    • 1
  1. 1.Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes of Ministry of Education, College of EnvironmentHohai UniversityNanjingChina
  2. 2.State Key Laboratory of Urban Water Resource and EnvironmentHarbin Institute of TechnologyHarbinChina

Personalised recommendations