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In situ anodic induction of low-valence copper in electro-Fenton system for effective nitrobenzene degradation

  • Yunting Wang
  • Gong Zhang
  • Yudong XueEmail author
  • Jiawei Tang
  • Xuelu Shi
  • Chunhui ZhangEmail author
Research Article
  • 36 Downloads

Abstract

To achieve superior advanced oxidation processes (AOPs), transitional state activators are of great significance for the production of active radicals by H2O2, while instability limits their activation efficiency. In this study, density functional theory calculation (DFT) results showed that Cu+ exhibits excellent H2O2 activation performance, with Gibbs free energy change (ΔG) of 33.66 kcal/mol, two times less than that of Cu2+ (77.83 kcal/mol). Meanwhile, an electro-Fenton system using Cu plate as an anode was proposed for in situ generation of Cu+. The released Cu with low-valence state can be well-confined on the surface of the exciting electrode, which was confirmed by X-ray photoelectron spectroscopy (XPS), Raman, and UV-vis spectroscopy. The hydroxyl radicals in this Cu-based electro-Fenton system were determined by the electron spin resonance (ESR). The nitrobenzene degradation ratio was greatly increased by 43.90% with the introduction of the proposed in situ electrochemical Cu+ generation process. Various characterization results indicated that the production of Cu+ was the key factor in the highly efficient Cu-based electro-Fenton reaction.

Keywords

Electrochemical advanced oxidation processes Transitional state Copper Electro-Fenton Nitrobenzene 

Notes

Funding information

This research was financially supported by the Research Fund of Major Science and Technology Program for Water Pollution Control and Treatment (2017ZX07402001).

Supplementary material

11356_2019_6387_MOESM1_ESM.pdf (373 kb)
ESM 1 (PDF 372 kb)

References

  1. Ai Z, Xia H, Mei T, Liu J, Zhang L, Deng K, Qiu J (2008) Electro-Fenton degradation of Rhodamine B based on a composite cathode of Cu2O nanocubes and carbon nanotubes. J Phys Chem C 112:11929–11935CrossRefGoogle Scholar
  2. Bai J, Liu Y, Yin X, Duan H, Ma J (2017) Efficient removal of nitrobenzene by Fenton-like process with Co-Fe layered double hydroxide. Appl Surf Sci 416:45–50CrossRefGoogle Scholar
  3. Bañuelos JA, García-Rodríguez O, Rodríguez-Valadez FJ, Godínez LA (2015) Electrochemically prepared iron-modified activated carbon electrodes for their application in electro-Fenton and photoelectro-Fenton processes. J Electrochem Soc 162:E154–E159CrossRefGoogle Scholar
  4. Bokare AD, Choi W (2014) Review of iron-free Fenton-like systems for activating H2O2 in advanced oxidation processes. J Hazard Mater 275:121–135CrossRefGoogle Scholar
  5. Chen F, Zhao X, Liu H, Qu J (2014) Enhanced destruction of Cu(CN)3 2− by H2O2 under alkaline conditions in the presence of EDTA/pyrophosphate. Chem Eng J 253:478–485CrossRefGoogle Scholar
  6. Choi K, Lee W (2012) Enhanced degradation of trichloroethylene in nano-scale zero-valent iron Fenton system with Cu(II). J Hazard Mater 211-212:146–153CrossRefGoogle Scholar
  7. Chumakov A, Batalova V, Slizhov Y (2016) Electro-Fenton-like reactions of transition metal ions with electrogenerated hydrogen peroxide. Am Inst Phys 1772:040004Google Scholar
  8. Costa RC, Lelis MF, Oliveira LC, Fabris JD, Ardisson JD, Rios RR, Silva CN, Lago RM (2006) Novel active heterogeneous Fenton system based on Fe3-xMxO4 (Fe, Co, Mn, Ni): the role of M2+ species on the reactivity towards H2O2 reactions. J Hazard Mater 129:171–178CrossRefGoogle Scholar
  9. Delley B (1990) An allelectron numerical method for solving the local density functional for polyatomic molecules. J Chem Phys 92:508–517CrossRefGoogle Scholar
  10. Delley B (2000) From molecules to solids with the DMol3 approach. J Chem Phys 113:7756–7764CrossRefGoogle Scholar
  11. Expósito E, Sánchez-Sánchez CM, Montiel V (2007) Mineral iron oxides as iron source in electro-Fenton and photoelectro-Fenton mineralization processes. J Electrochem Soc 154:E116–E122CrossRefGoogle Scholar
  12. Gabriel J, Shah V, Nesměrák K, Baldrian P, Nerud F (2000) Degradation of polycyclic aromatic hydrocarbons by the copper(II)-hydrogen peroxide system. Folia Microbiol 45:573–575CrossRefGoogle Scholar
  13. Gogate PR, Pandit AB (2004) A review of imperative technologies for wastewater treatment I: oxidation technologies at ambient conditions. Adv Environ Res 8:501–551CrossRefGoogle Scholar
  14. Guimaraes IR, Giroto A, Oliveira Luiz CA, Guerreiro MC, Lima DQ, Fabris JD (2009) Synthesis and thermal treatment of Cu-doped goethite: oxidation of quinoline through heterogeneous fenton process. Appl Catal B Environ 91:581–586CrossRefGoogle Scholar
  15. Hajimammadov R, Csendes Z, Ojakoski J-M, Lorite GS, Mohl M, Kordas K (2017) Nonlinear electronic transport and enhanced catalytic behavior caused by native oxides on Cu nanowires. Surf Sci 663:16–22CrossRefGoogle Scholar
  16. Hu Y, Li Y, He J, Liu T, Zhang K, Huang X, Kong L, Liu J (2018) EDTA-Fe(III) Fenton-like oxidation for the degradation of malachite green. J Environ Manag 226:256–263CrossRefGoogle Scholar
  17. Jiang J, Li G, Li Z, Zhang X, Zhang F (2016) An Fe–Mn binary oxide (FMBO) modified electrode for effective electrochemical advanced oxidation at neutral pH. Electrochim Acta 194:104–109CrossRefGoogle Scholar
  18. 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
  19. Li CW, Kanan MW (2012) CO2 reduction at low overpotential on Cu electrodes resulting from the reduction of thick Cu2O films. J Am Chem Soc 134:7231–7234CrossRefGoogle Scholar
  20. Li Y, Zhou W, Wang H, Xie L, Liang Y, Wei F, Idrobo JC, Pennycook SJ, Dai H (2012) An oxygen reduction electrocatalyst based on carbon nanotube-graphene complexes. Nat Nanotechnol 7:394–400CrossRefGoogle Scholar
  21. Li Y, Liu L, Liu L, Liu Y, Zhang H, Han X (2016) Efficient oxidation of phenol by persulfate using manganite as a catalyst. J Mol Catal A Chem 411:264–271CrossRefGoogle Scholar
  22. Liao P, Keith JA, Carter EA (2012) Water oxidation on pure and doped hematite (0001) surfaces: prediction of Co and Ni as effective dopants for electrocatalysis. J Am Chem Soc 134:13296–13309CrossRefGoogle Scholar
  23. Magalhães F, Pereira MC, Botrel SEC, Fabris JD, Macedo WA, Mendonça R, Lago RM, Oliveira LCA (2007) Cr-containing magnetites Fe3−xCrxO4: the role of Cr3+ and Fe2+ on the stability and reactivity towards H2O2 reactions. Appl Catal A Gen 332:115–123CrossRefGoogle Scholar
  24. Moreira AH, Benedetti AV, Cabot PL, Sumodjo TA (1993) Electrochemical behaviour of copper electrode in concentrated sulfuric acid solutions. Electrochim Acta 38:981–987CrossRefGoogle Scholar
  25. Moreira FC, Boaventura RAR, Brillas E, VJP V (2017) Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Appl Catal B Environ 202:217–262CrossRefGoogle Scholar
  26. Nguyen DCT, Oh WC (2018) Ternary self-assembly method of mesoporous silica and Cu2O combined graphene composite by nonionic surfactant and photocatalytic degradation of cationic-anionic dye pollutants. Sep Purif Technol 190:77–89CrossRefGoogle Scholar
  27. Nidheesh PV, Gandhimathi R (2014) Effect of solution pH on the performance of three electrolytic advanced oxidation processes for the treatment of textile wastewater and sludge characteristics. RSC Adv 4:27946CrossRefGoogle Scholar
  28. Nie Y, Hu C, Qu J, Zhao X (2009) Photoassisted degradation of endocrine disruptors over CuOx–FeOOH with H2O2 at neutral pH. Appl Catal B Environ 87:30–36CrossRefGoogle Scholar
  29. Peng J, Li J, Shi H, Wang Z, Gao S (2016) Oxidation of disinfectants with Cl-substituted structure by a Fenton-like system Cu2+/H2O2 and analysis on their structure-reactivity relationship. Environ Sci Pollut Res 23:1898–1904CrossRefGoogle Scholar
  30. Pérez-Moya M, Graells M, Buenestado P, Mansilla HD (2008) A comparative study on the empirical modeling of photo-Fenton treatment process performance. Appl Catal B Environ 84:313–323CrossRefGoogle Scholar
  31. Pignatello JJ, Oliveros E, MacKay A (2006) Advanced oxidation processes for organic contaminant destruction based on the Fenton reaction and related chemistry. Crit Rev Environ Sci Technol 36:1–84CrossRefGoogle Scholar
  32. Ramirez-Pereda B, Alvarez-Gallegos A, Rangel-Peraza JG, Bustos-Terrones YA (2018) Kinetics of Acid Orange 7 oxidation by using carbon fiber and reticulated vitreous carbon in an electro-Fenton process. J Environ Manag 213:279–287CrossRefGoogle Scholar
  33. Razgoniaev AO, McCusker CE, Castellano FN, Ostrowski AD (2017) Restricted photoinduced conformational change in the Cu(I) complex for sensing mechanical properties. ACS Macro Lett 6:920–924CrossRefGoogle Scholar
  34. Robbins M, Drago RS (1997) Activation of hydrogen peroxide for oxidation by copper(II) complexes. J Catal 170:295–303CrossRefGoogle Scholar
  35. Salem IA (2000) Kinetics of the oxidative color removal and degradation of bromophenol blue with hydrogen peroxide catalyzed by copper(II)-supported alumina and zirconia. Appl Catal B Environ 28:153–162CrossRefGoogle Scholar
  36. Santana-Martínez G, Roa-Morales G, Martin del Campo E, Romero R, Frontana-Uribe BA, Natividad R (2016) Electro-Fenton and electro-Fenton-like with in situ electrogeneration of H2O2 and catalyst applied to 4-chlorophenol mineralization. Electrochim Acta 195:246–256CrossRefGoogle Scholar
  37. Silva AC, Oliveira DQL, Oliveira LCA, Anastácio AS, Ramalho TC, Lopes JH, Carvalho HWP, Torres CER (2009) Nb-containing hematites Fe2−xNbxO3: the role of Nb5+ on the reactivity in presence of the H2O2 or ultraviolet light. Appl Catal A Gen 357:79–84CrossRefGoogle Scholar
  38. Singh A, Verma A, Bansal P, Singla J (2017) Evaluation of the process parameters for electro Fenton and electro chlorination treatment of Reactive Black 5 (RB5) dye. J Electrochem Soc 164:E203–E212CrossRefGoogle Scholar
  39. Tahir D, Tougaard S (2012) Electronic and optical properties of Cu, CuO and Cu2O studied by electron spectroscopy. J Phys Condens Matter 24:175002CrossRefGoogle Scholar
  40. Verma P, Baldrian P, Gabriel J, Trnka T, Nerud F (2004) Copper–ligand complex for the decolorization of synthetic dyes. Chemosphere 57:1207–1211CrossRefGoogle Scholar
  41. Wang A, Cheng H, Liang B, Ren N, Cui D, Lin N, Kim BH, Rabaey K (2011) Efficient reduction of nitrobenzene to aniline with a biocatalyzed cathode. Environ Sci Technol 45:10186–10193CrossRefGoogle Scholar
  42. Wang J, Liu C, Tong L, Li J, Luo R, Qi J, Li Y, Wang L (2015) Iron–copper bimetallic nanoparticles supported on hollow mesoporous silica spheres: an effective heterogeneous Fenton catalyst for orange II degradation. RSC Adv 5:69593–69605CrossRefGoogle Scholar
  43. Wang Y, Ji Z, Shen X, Zhu G, Wang J, Yue X (2017) Facile growth of Cu2O hollow cubes on reduced graphene oxide with remarkable electrocatalytic performance for non-enzymatic glucose detection. New J Chem 41:9223–9229CrossRefGoogle Scholar
  44. Wang Y, Xue Y, Zhang C (2019) Enhanced anodic dissolution of cupronickel alloy scraps by electro-generated reactive oxygen species in acid media. J Alloys Compd 806:106–112CrossRefGoogle Scholar
  45. Xu X, Liao P, Yuan S, Tong M, Luo M, Xie W (2013) Cu-catalytic generation of reactive oxidizing species from H2 and O2 produced by water electrolysis for electro-fenton degradation of organic contaminants. Chem Eng J 233:117–123CrossRefGoogle Scholar
  46. Xue Y, Jin W, Du H, Zheng S, Sun Z, Yan W, Zhang Y (2016) Electrochemical Cr(III) oxidation and mobilization by in situ generated reactive oxygen species in alkaline solution. J Electrochem Soc 163:H684–H689CrossRefGoogle Scholar
  47. Xue Y, Zhang Y, Zhang Y, Zheng S, Zhang Y, Jin W (2017a) Electrochemical detoxification and recovery of spent SCR catalyst by in-situ generated reactive oxygen species in alkaline media. Chem Eng J 325:544–553CrossRefGoogle Scholar
  48. Xue Y, Zheng S, Du H, Zhang Y, Jin W (2017b) Cr(III)-induced electrochemical advanced oxidation processes for the V2O3 dissolution in alkaline media. Chem Eng J 307:518–525CrossRefGoogle Scholar
  49. Xue Y, Zheng S, Sun Z, Zhang Y, Jin W (2017c) Alkaline electrochemical advanced oxidation process for chromium oxidation at graphitized multi-walled carbon nanotubes. Chemosphere 183:156–163CrossRefGoogle Scholar
  50. Yang S, He H, Wu D, Chen D, Liang X, Qin Z, Fan M, Zhu J, Yuan P (2009) Decolorization of methylene blue by heterogeneous Fenton reaction using Fe3−xTixO4 (0 ≤ x ≤ 0.78) at neutral pH values. Appl Catal B Environ 89:527–535CrossRefGoogle Scholar
  51. Zhang G, Gao Y, Zhang Y, Guo Y (2010) Fe2O3-pillared rectorite as an efficient andstable Fenton-like heterogeneous catalyst for photodegradation of organiccontaminants. Environ Sci Technol 44:6384–6389CrossRefGoogle Scholar
  52. Zhang G, Wang S, Zhao S, Fu L, Chen G, Yang F (2011) Oxidative degradation of azo dye by hydrogen peroxide electrogenerated in situ on anthraquinonemonosulphonate/polypyrrole composite cathode with heterogeneous CuO/γ-Al2O3 catalyst. Appl Catal B Environ 106:370–378CrossRefGoogle Scholar
  53. Zhang L, Nie Y, Hu C, Qu J (2012) Enhanced Fenton degradation of Rhodamine B over nanoscaled Cu-doped LaTiO3 perovskite. Appl Catal B Environ 125:418–424CrossRefGoogle Scholar
  54. Zhang Q, Liu Y, Chen S, Quan X, Yu H (2014) Nitrogen-doped diamond electrode shows high performance for electrochemical reduction of nitrobenzene. J Hazard Mater 265:185–190CrossRefGoogle Scholar
  55. Zhao L, Ma J, Sun Z (2008) Oxidation products and pathway of ceramic honeycomb-catalyzed ozonation for the degradation of nitrobenzene in aqueous solution. Appl Catal B Environ 79:244–253CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.School of Chemical and Environmental EngineeringChina University of Mining and Technology of BeijingBeijingPR China
  2. 2.Center for Water and Ecology, State Key Joint Laboratory of Environment Simulation and Pollution Control, School of EnvironmentTsinghua UniversityBeijingPR China
  3. 3.National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, CAS Key Laboratory of Green Process and Engineering, Institute of Process EngineeringChinese Academy of SciencesBeijingPR China

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