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Enhancement of the electrocatalytic oxidation of dyeing wastewater (reactive brilliant blue KN-R) over the Ce-modified Ti-PbO2 electrode with surface hydrophobicity

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Abstract

Rational hydrophobic anode has been considered as a promising approach for water pollution remediation. However, the construction method of the hydrophobic electrode is limited, such as adding hydrophobic polymer materials. Herein, we address this limitation by developing Ce-modified Ti-PbO2 electrodes with distinctive micro/nanostructures and surface hydrophobicity by the typical electro-deposition process. The Pb ions in the lattice of PbO2 crystals can be substituted by cerium ions and the PbO2 crystal grains were refined when the concentration of cerium ions is low. Specifically, as further increase of the cerium content in plating solution, the CeO2 gradually precipitated on the surface of PbO2 and the PbO2 phase was becoming more and more amorphous. Namely, the pyramid structure converted to surface outshoots with outward oriented-growth, and then evolved gradually to branched projections, until the coral-like architecture was constructed by assembling of small particles. More importantly, the micro/nanostructures and surface hydrophobic PbO2 coatings can significantly enhance generating and utilizing efficiency of hydroxyl radicals, charge transfer rate, and electrochemical active area. The excellent electrochemical performance is mainly attributed to superior catalytic activity arises from synergetic effects between cerium and PbO2 and distinctive micro/nanostructures hydrophobicity surface of Ce-modified Ti-PbO2 electrodes.

Graphical abstract

A novel Ce-modified Ti-PbO2 electrode with distinctive micro/nanostructures and surface hydrophobicity was fabricated by the typical electro-deposition process. The as-prepared Ce-modified Ti-PbO2 electrode possesses high generating and utilizing efficiency of hydroxyl radicals, fast charge transfer, and large electrochemical active area due to its higher OEP, lower charge transfer resistance, higher carrier density (ND value), and stronger surface hydrophobicity. Consequently, the Ce-modified Ti-PbO2 electrode exhibited better electro-oxidation performance for removing reactive brilliant blue KN-R, as compared with that of Ti-PbO2-reference (without Ce modifying).

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References

  1. Buthiyappan A, Abdul Aziz AR, Wan Daud WMA (2016) Recent advances and prospects of catalytic advanced oxidation process in treating textile effluents. Rev Chem Eng 32(1):1–47

    Article  CAS  Google Scholar 

  2. Korbahti BK, Tanyolac A (2008) Electrochemical treatment of simulated textile wastewater with industrial components and levafix blue ca reactive dye: optimization through response surface methodology. J Hazard Mater 151(2-3):422–431

    Article  CAS  PubMed  Google Scholar 

  3. Li X, Li X, Yang W, Chen X, Li W, Luo B, Wang K (2014) Preparation of 3D PbO2 nanospheres@SnO2 nanowires/Ti electrode and its application in methyl orange degradation. Electrochim Acta 146:15–22

    Article  CAS  Google Scholar 

  4. Zhang S, Lu X (2018) Treatment of wastewater containing reactive brilliant blue KN-R using TiO2/BC composite as heterogeneous photocatalyst and adsorbent. Chemosphere 206:777–783

    Article  CAS  PubMed  Google Scholar 

  5. Gurung K, Ncibi MC, Shestakova M, Sillanpaa M (2018) Removal of carbamazepine from MBR effluent by electrochemical oxidation (EO) using a Ti/Ta2O5-SnO2 electrode. Appl Catal B 221:329–338

    Article  CAS  Google Scholar 

  6. Duan X, Xu F, Wang Y, Chen Y, Chang L (2018) Fabrication of a hydrophobic SDBS-PbO2 anode for electrochemical degradation of nitrobenzene in aqueous solution. Electrochim Acta 282:662–671

    Article  CAS  Google Scholar 

  7. Wang C, Li J, Mele G, Yang GM, Zhang FX, Palmisano L, Vasapollo G (2007) Efficient degradation of 4-nitrophenol by using functionalized porphyrin-TiO2 photocatalysts under visible irradiation. Appl Catals B 76(3-4):218–226

    Article  CAS  Google Scholar 

  8. Priya MH, Madras G (2006) Photocatalytic degradation of nitrobenzenes with combustion synthesized nano-TiO2. J Photochem Photobiol A 178(1):1–7

    Article  CAS  Google Scholar 

  9. Rozendal RA, Hamelers HV, Rabaey K, Keller J, Buisman CJ (2008) Towards practical implementation of bioelectrochemical wastewater treatment. Trends Biotechnol 26(8):450–459

    Article  CAS  PubMed  Google Scholar 

  10. Kou T, Jin C, Zhang C, Sun J, Zhang Z (2012) Nanoporous core–shell cu@Cu2O nanocomposites with superior photocatalytic properties towards the degradation of methyl orange. RSC Adv 2(33):12636

    Article  CAS  Google Scholar 

  11. Xia X, Tu J, Zhang Y, Chen J, Wang X, Gu C, Guan C, Luo J, Fan HJ (2012) Porous hydroxide nanosheets on preformed nanowires by electrodeposition: branched nanoarrays for electrochemical energy storage. Chem Mater 24(19):3793–3799

    Article  CAS  Google Scholar 

  12. Zhao Y, Ran W, He J, Song Y, Zhang C, Xiong DB, Gao F, Wu J, Xia Y (2015) Oxygen-rich hierarchical porous carbon derived from artemia cyst shells with superior electrochemical performance. ACS Appl Mater Interfaces 7(2):1132–1139

    Article  CAS  PubMed  Google Scholar 

  13. Wang Y, Song Y, Xia Y (2016) Electrochemical capacitors: mechanism, materials, systems, characterization and applications. Chem Soc Rev 45(21):5925–5950

    Article  CAS  PubMed  Google Scholar 

  14. Wu Z, Li W, Xia Y, Webley P, Zhao D (2012) Ordered mesoporous graphitized pyrolytic carbon materials: synthesis, graphitization, and electrochemical properties. J Mater Chem 22(18):8835

    Article  CAS  Google Scholar 

  15. Ye Z, Li T, Ma G, Peng X, Zhao J (2017) Morphology controlled MnO2 electrodeposited on carbon fiber paper for high-performance supercapacitors. J Power Sources 351:51–57

    Article  CAS  Google Scholar 

  16. Wang W, Fan X, Qin Y, Liu J, Yan C, Zeng C (2018) The reduction reaction kinetics of vanadium (V) in acidic solutions on a platinum electrode with unusual difference compared to carbon electrodes. Electrochim Acta 283:1313–1322

    Article  CAS  Google Scholar 

  17. Panic VV, Dekanski AB, Vidakovic TR, Miskovic Stankovic VB, Javanovic BZ, Nikolic BZ (2004) Oxidation of phenol on RuO2-TiO2/Ti anodes. J Solid State Electrochem 9:43–54

    Article  CAS  Google Scholar 

  18. Rodgers JD, Jedral W, Bunce NJ (1999) Electrochemical oxidation of chlorinated phenols. Environ Sci Technol 33(9):1453–1457

    Article  CAS  Google Scholar 

  19. Ma D, Li Y, Mi H, Luo S, Zhang P, Lin Z, Li J, Zhang H (2018) Robust SnO2-x nanoparticle-impregnated carbon nanofibers with outstanding electrochemical performance for advanced sodium-ion batteries. Angew Chem Int Ed 57(29):8901–8905

    Article  CAS  Google Scholar 

  20. Yang B, Wang J, Jiang C, Li J, Yu G, Deng S, Lu S, Zhang P, Zhu C, Zhuo Q (2017) Electrochemical mineralization of perfluorooctane sulfonate by novel F and Sb co-doped Ti/SnO2 electrode containing Sn-Sb interlayer. Chem Eng J 316:296–304

    Article  CAS  Google Scholar 

  21. Phillips RB, James RR, Magnuson ML (2018) Electrolyte selection and microbial toxicity for electrochemical oxidative water treatment using a boron-doped diamond anode to support site specific contamination incident response. Chemosphere 197:135–141

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  22. Comninellis C (1994) Electrocatalysis in the electrochemical conversion/combustion of organic pollutants for waste water treatment. Electrochim Acta 39(11-12):1857–1862

    Article  CAS  Google Scholar 

  23. Song F, Hu X (2014) Ultrathin cobalt-manganese layered double hydroxide is an efficient oxygen evolution catalyst. J Am Chem Soc 136(47):16481–16484

    Article  CAS  PubMed  Google Scholar 

  24. Martinez-Huitle CA, Brillas E (2009) Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods: a general review. Appl Catal, B 87(3-4):105–145

    Article  CAS  Google Scholar 

  25. Martinez-Huitle CA, Ferro S (2006) Electrochemical oxidation of organic pollutants for the wastewater treatment: direct and indirect processes. Chem Soc Rev 35(12):1324–1340

    Article  CAS  PubMed  Google Scholar 

  26. Li X, Pletcher D, Walsh FC (2011) Electrodeposited lead dioxide coatings. Chem Soc Rev 40(7):3879–3894

    Article  CAS  PubMed  Google Scholar 

  27. Qiao Q, Singh S, Lo S-L, Li Y, Jin J, Wang L (2018) Electrochemical oxidation of acid orange 7 dye with Ce, Nd, and Co-modified PbO2 electrodes: preparation, characterization, optimization, and mineralization. J Taiwan Inst Chem Eng 84:110–122

    Article  CAS  Google Scholar 

  28. Liu Y, Liu H, Ma J, Li J (2011) Investigation on electrochemical properties of cerium doped lead dioxide anode and application for elimination of nitrophenol. Electrochim Acta 56(3):1352–1360

    Article  CAS  Google Scholar 

  29. Wang Z, Xu M, Wang F, Liang X, Wei Y, Hu Y, Zhu CG, Fang W (2017) Preparation and characterization of a novel Ce doped PbO2 electrode based on NiO modified Ti/TiO2NTs substrate for the electrocatalytic degradation of phenol wastewater. Electrochim Acta 247:535–547

    Article  CAS  Google Scholar 

  30. Yao Y, Zhao M, Zhao C, Ma L (2014) Influence of duty cycle on the structure and electrocatalyticproperties of pulse electrodeposited lead dioxide electrodes. J Solid State Electrochem 18(3):721–727

    Article  CAS  Google Scholar 

  31. Hu X, Yu Y, Yang L (2015) Electrocatalytic activity of Ce-PbO2/C anode for acid red B reduction in aqueous solution. J Solid State Electrochem 19(6):1599–1609

    Article  CAS  Google Scholar 

  32. Du H, Duan G, Wang N, Liu J, Tang Y, Pang R, Chen Y, Wan P (2018) Fabrication of Ga2O3–PbO2 electrode and its performance in electrochemical advanced oxidation processes. J Solid State Electrochem 22(12):3799–3806

    Article  CAS  Google Scholar 

  33. Zaidi SZJ, Harito C, Walsh FC, Ponce de Leon C (2018) Decolourisation of reactive black-5 at an RVC substrate decorated with PbO2/TiO2 nanosheets prepared by anodic electrodeposition. J Solid State Electrochem 22(9):2889–2900

    Article  CAS  Google Scholar 

  34. Pereira JF, Figueiredo RS, Ponce-de-Leon C, Bertazzoli R (2016) Platinum-free lead dioxide electrode for electrooxidation of organic compounds. J Solid State Electrochem 20(4):1167–1173

    Article  CAS  Google Scholar 

  35. Santos J E L, de Moura D C, da Silva D R, Panizza M, Martinez-Huitle C A (2018) Application of TiO2-nanotubes/PbO2 as an anode for the electrochemical elimination of acid red 1 dye. J Solid State Electrochem 1-10

  36. Velichenko AB, Amadelli R, Gruzdeva EV, Luk’yanenko TV, Danilov FI (2009) Electrodeposition of lead dioxide from methanesulfonate solutions. J Power Sources 191(1):103–110

    Article  CAS  Google Scholar 

  37. Tang Z, Lu G (2006) High performance rare earth oxides LnOx (Ln= Sc, Y, La, Ce, Pr and Nd) modified Pt/C electrocatalysts for methanol electrooxidation. J Power Sources 162(2):1067–1072

    Article  CAS  Google Scholar 

  38. Fernandes KC, Silva LMD, Boodts JFC, De Faria LA (2006) Surface, kinetics and electrocatalytic properties of the Ti/(Ti+ Ru+ Ce) O2-system for the oxygen evolution reaction in alkaline medium. Electrochim Acta 51(14):2809–2818

    Article  CAS  Google Scholar 

  39. Da Silva LM, Fernandes KC, De Faria LA, Boodts JFC (2004) Electrochemical impedance spectroscopy study during accelerated life test of conductive oxides: Ti/(Ru+ Ti+ Ce) O2-system. Electrochim Acta 49(27):4893–4906

    Article  CAS  Google Scholar 

  40. De Faria LA, Boodts JFC, Trasatti S (1997) Electrocatalytic properties of Ru+Ti+Ce mixed oxide electrodes for the Cl2 evolution reaction. Electrochim Acta 42(23-24):3525–3530

    Article  Google Scholar 

  41. Kou T, Si C, Pinto J, Ma C, Zhang Z (2017) Dealloying assisted high-yield growth of surfactant-free <110> highly active Cu-doped CeO2 nanowires for low-temperature CO oxidation. Nanoscale 9(23):8007–8014

    Article  CAS  PubMed  Google Scholar 

  42. Kong J, Shi S, Kong L, Zhu X, Ni J (2007) Preparation and characterization of PbO2 electrodes doped with different rare earth oxides. Electrochim Acta 53(4):2048–2054

    Article  CAS  Google Scholar 

  43. Ai S, Gao M, Zhang W, Wang Q, Xie Y, Jin L (2004) Preparation of Ce-PbO2 modified electrode and its application in detection of anilines. Talanta 62(3):445–450

    Article  CAS  PubMed  Google Scholar 

  44. Shmychkova O, Luk’yanenko T, Velichenko A, Meda L, Amadelli R (2013) Bi-doped PbO2 anodes: electrodeposition and physico-chemical properties. Electrochim Acta 111:332–338

    Article  CAS  Google Scholar 

  45. Wooh S, Encinas N, Vollmer D, Butt HJ (2017) Stable hydrophobic metal-oxide photocatalysts via grafting polydimethylsiloxane brush. Adv Mater 29(16)

  46. Li Y, Zhao C (2017) Enhancing water oxidation catalysis on a synergistic phosphorylated nife hydroxide by adjusting catalyst wettability. ACS Catal 7(4):2535–2541

    Article  CAS  Google Scholar 

  47. Zhao G, Zhang Y, Lei Y, Lv B, Gao J, Zhang Y, Li D (2010) Fabrication and electrochemical treatment application of a novel lead dioxide anode with superhydrophobic surfaces, high oxygen evolution potential, and oxidation capability. Environ Sci Technol 44(5):1754–1759

    Article  CAS  PubMed  Google Scholar 

  48. Yu HB, Song YN, Zhao B, Lu Y, Zhu SY, Qu J, Wang XH, Qin WC (2018) Efficient electrocatalytic degradation of 4-Chlorophenol using a Ti/RuO2–SnO2–TiO2/PbO2–CeO2 composite electrode. Electrocatalysis 9(6):725–734

    Article  CAS  Google Scholar 

  49. Yao YW, Jiao LM, Cui LH, Yu NC, Wei F, Lu ZM (2015) Preparation and characterization of PbO2-CeO2 nanocomposite electrode with high cerium content and its appplication in the electrocatalytic degradation of malachite green. J Electrochem Soc 162(9):H693–H698

    Article  CAS  Google Scholar 

  50. Velichenko AB, Amadelli R, Benedetti A, Girendko DV, Kovalyov SV, Danilov FI (2002) Electrosynthesis and physicochemical properties of PbO2 films. J Electrochem Soc 149(9):C445–C449

    Article  CAS  Google Scholar 

  51. Velichenko AB, Devilliers D (2007) Electrodeposition of fluorine-doped lead dioxide. J Fluor Chem 128(4):269–276

    Article  CAS  Google Scholar 

  52. Zhang J, Yu J, Jaroniec M, Gong JR (2012) Noble metal-free reduced graphene oxide-ZnxCd1−xS nanocomposite with enhanced solar photocatalytic H2-production performance. Nano Lett 12(9):4584–4589

    Article  CAS  PubMed  Google Scholar 

  53. Li Q, Zhang Q, Cui H, Ding L, Wei Z, Zhai J (2013) Fabrication of cerium-doped lead dioxide anode with improved electrocatalytic activity and its application for removal of rhodamine B. Chem Eng J 228:806–814

    Article  CAS  Google Scholar 

  54. Qiu L, Liu F, Zhao L, Ma Y, Yao J (2006) Comparative XPS study of surface reduction for nanocrystalline and microcrystalline ceria powder. Appl Surf Sci 252(14):4931–4935

    Article  CAS  Google Scholar 

  55. Beche E, Charvin P, Perarnau D, Abanades S, Flamant G (2008) Ce 3d XPS investigation of cerium oxides and mixed cerium oxide (CexTiyOz). Surf Interface Anal 40(3-4):264–267

    Article  CAS  Google Scholar 

  56. Gao X, Jiang L (2004) Water-repellent legs of water striders. Nature 432(7013):36

    Article  CAS  PubMed  Google Scholar 

  57. Wooh S, Encinas N, Vollmer D, Butt HJ (2017) Stable hydrophobic metal-oxide photocatalysts via grafting polydimethylsiloxane brush. Adv Mater 29(16):1604637

    Article  CAS  Google Scholar 

  58. Sheng X, Liu Z, Zeng R, Chen L, Feng X, Jiang L (2017) Enhanced photocatalytic reaction at air-liquid-solid joint interfaces. J Am Chem Soc 139(36):12402–12405

    Article  CAS  PubMed  Google Scholar 

  59. Zhang L, Xu L, He J, Zhang J (2014) Preparation of Ti/SnO2-Sb electrodes modified by carbon nanotube for anodic oxidation of dye wastewater and combination with nanofiltration. Electrochim Acta 117:192–201

    Article  CAS  Google Scholar 

  60. Hao X, Wuqi G, Jia W, Jiangtao F, Honghui Y, Wei Y (2016) Preparation and characterization of titanium-based PbO2 electrodes modified by ethylene glycol. RSC Adv 6(9):7610–7617

    Article  CAS  Google Scholar 

  61. Hao X, Dan S, Qian Z, Honghui Y, Yan W (2014) Preparation and characterization of PbO2 electrodes from electro-deposition solutions with different copper concentration. RSC Adv 4(48):25011

    Article  CAS  Google Scholar 

  62. Wang Z, Yang C, Lin T, Yin H, Chen P, Wan D, Xu F, Huang F, Lin J, Xie X, Jiang M (2013) Visible-light photocatalytic, solar thermal and photoelectrochemical properties of aluminium-reduced black titania. Energy Environ Sci 6(10):3007

    Article  CAS  Google Scholar 

  63. Huang Z, Liu J, Xiao Z, Fu H, Fan W, Xu B, Dong B, Liu D, Dai F, Sun D (2018) A MOF-derived coral-like NiSe@NC nanohybrid: an efficient electrocatalyst for the hydrogen evolution reaction at all pH values. Nanoscale https://doi.org/10.1039/C8NR06877A

  64. Harrington SP, Devine TM (2008) Analysis of electrodes displaying frequency dispersion in Mott-schottky tests. J Electrochem Soc 155(8):C381–C386

    Article  CAS  Google Scholar 

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Funding

This work was supported by the National Natural Science Foundation of China (21875026, 21878031), the Program for Liaoning Excellent Talents in University (LR2014013), and the Science and Technology Foundation of Liaoning Province (No. 201602052).

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Correspondence to Hongchao Ma or Yinghuan Fu.

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Highlights

•The surface micro/nanostructures of PbO2 coatings can be tailored by adding Ce.

•The surface hydrophobicity of PbO2 coatings arises from itself distinctive micro/nanostructures.

•The precipitation of CeO2 on the PbO2 surface is key factor to construct distinctive micro/nanostructures.

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Lyu, J., Han, H., Wu, Q. et al. Enhancement of the electrocatalytic oxidation of dyeing wastewater (reactive brilliant blue KN-R) over the Ce-modified Ti-PbO2 electrode with surface hydrophobicity. J Solid State Electrochem 23, 847–859 (2019). https://doi.org/10.1007/s10008-018-04170-9

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  • DOI: https://doi.org/10.1007/s10008-018-04170-9

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