Abstract
In this study, binary and ternary mixed metal oxide anodes of Ti/RuO2–Sb2O4 and Ti/RuO2–Sb2O4–TiO2 were prepared using two different heating methods: conventional furnace and alternative CO2 laser heating. The produced anodes were physically and electrochemically characterized by using different techniques. The main difference found in the laser-made anodes was their more compact morphology, without the common deep cracks found in anodes made by typical thermal decomposition, which showed an important correlation with the prolonged accelerated service life. The correlation between the physicochemical properties of the anodes with their performance towards the 4-nitrophenol oxidations is discussed. The results demonstrated that the ternary anode (Ti/RuO2–Sb2O4–TiO2) is very promising, presenting a kinetic 5.7 times faster than the respective binary anode and the highest removal efficiency when compared with conventionally made anodes. Also, the lowest energy consumption per unit of mass of contaminant removed is seen for the laser-made Ti/RuO2–Sb2O4–TiO2 anode, which evidences the excellent cost–benefit of this anode material. Finally, some by-products were identified, and a degradation route is proposed.
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Acosta-Santoyo G, Llanos J, Raschitor A, Bustos E, Cañizares P, Rodrigo MA (2020) Performance of ultrafiltration as a pre-concentration stage for the treatment of oxyfluorfen by electrochemical BDD oxidation. Sep Purif Technol 237:116366. https://doi.org/10.1016/j.seppur.2019.116366
Ahn W-Y, Sheeley SA, Rajh T, Cropek DM (2007) Photocatalytic reduction of 4-nitrophenol with arginine-modified titanium dioxide nanoparticles. Appl Catal B Environ 74:103–110. https://doi.org/10.1016/j.apcatb.2007.01.016
Audichon T, Napporn TW, Canaff C, Morais C, Comminges CM, Kokoh KB (2016) IrO2 coated on RuO2 as efficient and stable electroactive nanocatalysts for electrochemical water splitting. J Phys Chem C 120:2562–2573. https://doi.org/10.1021/acs.jpcc.5b11868
Berenguer R, Sieben JM, Quijada C, Morallón E (2016) Electrocatalytic degradation of phenol on Pt-and Ru-doped Ti/SnO2-Sb anodes in an alkaline medium. Appl Catal B-Environ 199:394–404. https://doi.org/10.1016/j.apcatb.2016.06.038
Bezerra CWA, Santos GOS, Pupo MMS, Gomes MA, Silva RS, Eguiluz KIB, Salazar-Banda GR (2020) Novel eco-friendly method to prepare Ti/RuO2–IrO2 anodes by using polyvinyl alcohol as the solvent. J Electroanal Chem 113822:113822. https://doi.org/10.1016/j.jelechem.2020.113822
Bi Q, Xue J, Tang C, Yu L, Li G, Zhang X (2016) The modification mechanism of lanthanum doping in Ti/Sb-SnO2 electrode and its electrocatalytic behavior of degradation of p-nitrophenol. Int J Electrochem Sci 11:7412–7429. https://doi.org/10.20964/2016.09.10
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 and Applied Chemistry 73:627–637
Cañizares P, Saez C, Lobato J, Rodrigo M (2004) Electrochemical treatment of 4-nitrophenol-containing aqueous wastes using boron-doped diamond anodes. Ind Eng Chem Res 43:1944–1951. https://doi.org/10.1021/ie034025t
Chalupczok S, Kurzweil P, Hartmann H, Schell C (2018) The redox chemistry of ruthenium dioxide: a cyclic voltammetry study—review and revision. Int J Electrochem 2018:1–15. https://doi.org/10.1155/2018/1273768
Comninellis C, Vercesi G (1991) Characterization of DSA®-type oxygen evolving electrodes: choice of a coating. J Appl Electrochem 21:335–345. https://doi.org/10.1007/BF01020219
Da Silva LA, Alves VA, da Silva MAP, Trasatti S, Boodts JFC (1997) Morphological, chemical, and electrochemical properties of Ti/(TiO2 + IrO2) electrodes. Can J Chem 75:1483–1493
Da Silva L, De Faria L, Boodts J (2001) Determination of the morphology factor of oxide layers. Electrochim Acta 47:395–403. https://doi.org/10.1016/S0013-4686(01)00738-1
Da Silva LM, Santos GOS, Pupo MMS, Eguiluz KIB, Salazar-Banda GR (2018) Influence of heating rate on the physical and electrochemical properties of mixed metal oxides anodes synthesized by thermal decomposition method applying an ionic liquid. J Electroanal Chem 813:127–133. https://doi.org/10.1016/j.jelechem.2018.02.026
Deblonde T, Cossu-Leguille C, Hartemann P (2011) Emerging pollutants in wastewater: a review of the literature. Int J Hyg Environ Health 214:442–448. https://doi.org/10.1016/j.ijheh.2011.08.002
Dória AR, Silva RS, Júnior PHO, dos Santos EA, Mattedi S, Hammer P, Salazar-Banda GR, Eguiluz KIB (2020) Influence of the RuO2 layer thickness on the physical and electrochemical properties of anodes synthesized by the ionic liquid method. Electrochim Acta:136625, Pre-proof. https://doi.org/10.1016/j.electacta.2020.136625
Duan X, Zhao Y, Liu W, Chang L, Li X (2014) Electrochemical degradation of p-nitrophenol on carbon nanotube and Ce-modified-PbO2 electrode. J Taiwan Inst Chem E 45:2975–2985. https://doi.org/10.1016/j.jtice.2014.08.031
Duan X, Li J, Chang L, Yang C (2016) A comparison of electrochemical oxidation performance of PbO2 and SnO2 electrodes. Journal of Water Reuse Desalination 6:392–398. https://doi.org/10.2166/wrd.2016.150
Ensano BMB, Borea L, Naddeo V, de Luna MDG, Belgiorno V (2019) Control of emerging contaminants by the combination of electrochemical processes and membrane bioreactors. Environ Sci Pollut R 26:1103–1112. https://doi.org/10.1007/s11356-017-9097-z
Fan J, Zhao G, Zhao H, Chai S, Cao T (2013) Fabrication and application of mesoporous Sb-doped SnO2 electrode with high specific surface in electrochemical degradation of ketoprofen. Electrochim Acta 94:21–29. https://doi.org/10.1016/j.electacta.2013.01.129
Garcia-Segura S, Brillas E (2016) Combustion of textile monoazo, diazo and triazo dyes by solar photoelectro-Fenton: decolorization, kinetics and degradation routes. Appl Catal B-Environ 181:681–691. https://doi.org/10.1016/j.apcatb.2015.08.042
Goudarzi M, Ghorbani M (2015) A study on ternary mixed oxide coatings containing Ti, Ru, Ir by sol–gel method on titanium. J Sol-Gel Sci Technol 73:332–340. https://doi.org/10.1007/s10971-014-3537-8
Guo Q, Qin X (2014) Flower-like SnO2 nanoparticles grown on graphene as anode materials for lithium-ion batteries. J Solid State Electr 18:1031–1039. https://doi.org/10.1007/s10008-013-2352-4
Jiang Y, Hu Z, Zhou M, Zhou L, Xi B (2014) Efficient degradation of p-nitrophenol by electro-oxidation on Fe doped Ti/TiO2 nanotube/PbO2 anode. Sep Purif Technol 128:67–71. https://doi.org/10.1016/j.seppur.2014.03.015
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. https://doi.org/10.1016/j.cej.2014.11.051
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. https://doi.org/10.1016/j.chemosphere.2017.08.145
Li G, Zhu M, Chen J, Li Y, Zhang X (2011) Production and contribution of hydroxyl radicals between the DSA anode and water interface. J Environ Sci 23(5):744–748. https://doi.org/10.1016/S1001-0742(10)60470-6
Lin KYA, Hsieh YT (2015) Copper-based metal organic framework (MOF), HKUST-1, as an efficient adsorbent to remove p-nitrophenol from water. J Taiwan Inst Chem E 50:223–228. https://doi.org/10.1016/j.jtice.2014.12.008
Llanos J, Raschitor A, Cañizares P, Rodrigo MA (2018) Exploring the applicability of a combined electrodialysis/electro-oxidation cell for the degradation of 2,4-dichlorophenoxyacetic acid. Electrochim Acta 269:415–421. https://doi.org/10.1016/j.electacta.2018.02.153
Majumdar D, Thandavarayan M, Zhongqing J (2019) Recent progress in ruthenium oxide-based composites for supercapacitor applications. ChemElectroChem 6(17):4343–4372. https://doi.org/10.1002/celc.201900668
Martínez-Huitle CA, Rodrigo MA, Sirés I, Scialdone O (2015) Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem Rev 115:13362–13407. https://doi.org/10.1021/acs.chemrev.5b00361
Mattos-Costa FI, de Lima-Neto P, Machado SAS, Avaca LA (1998) Characterisation of surfaces modified by sol-gel derived RuxIr1−xO2 coatings for oxygen evolution in acid medium. Electrochim Acta 44(8–9):1515–1523. https://doi.org/10.1016/S0013-4686(98)00275-8
Moradi F, Dehghanian C (2014) Addition of IrO2 to RuO2+ TiO2 coated anodes and its effect on electrochemical performance of anodes in acid media. Prof Nat Sci Mater Int 24:134–141. https://doi.org/10.1016/j.pnsc.2014.03.008
Muñoz M, Llanos J, Raschitor A, Cañizares P, Rodrigo MA (2017) Electrocoagulation as the key for an efficient concentration and removal of oxyfluorfen from liquid wastes. Ind Eng Chem Res 56(11):3091–3097. https://doi.org/10.1021/acs.iecr.7b00347
Murugaesan P, Aravind P, Muniyandi NG, Kandasamy S (2015) Performance of three different anodes in electrochemical degradation of 4-para-nitrophenol. Environ Technol 36:2618–2627. https://doi.org/10.1080/09593330.2015.1041424
Näslund LÅ, Sánchez-Sánchez CM, Ingason ÁS, Bäckström J, Herrero E, Rosen J, Holmin S (2013) The role of TiO2 doping on RuO2-coated electrodes for the water oxidation reaction. J Phys Chem 117(12):6126–6135. https://doi.org/10.1021/jp308941g
Padilla-Sánchez JA, Plaza-Bolanos P, Romero-González R, Barco-Bonilla N, Martínez-Vidal JL, Garrido-Frenich A (2011) Simultaneous analysis of chlorophenols, alkylphenols, nitrophenols and cresols in wastewater effluents, using solid phase extraction and further determination by gas chromatography–tandem mass spectrometry. Talanta 85(5):2397–2404. https://doi.org/10.1016/j.talanta.2011.07.081
Pushpavanam S, Narasimham K (1994) Morphology of (Ru-Ti-Sn) mixed-oxide coatings. J Mater Sci 29:939–942. https://doi.org/10.1007/BF00351413
Quiroz M, Reyna S, Martinez-Huitle C, Ferro S, De Battisti A (2005) Electrocatalytic oxidation of p-nitrophenol from aqueous solutions at Pb/PbO2 anodes. Appl Catal B-Environ 59:259–266. https://doi.org/10.1016/j.apcatb.2005.02.009
Rajkumar D, Kim JG (2006) Oxidation of various reactive dyes with in situ electro-generated active chlorine for textile dyeing industry wastewater treatment. J Hazard Mater 136:203–212. https://doi.org/10.1016/j.jhazmat.2005.11.096
Rao ANS, Venkatarangaiah V (2014) Metal oxide-coated anodes in wastewater treatment. Environ Sci Pollut R 21:3197–3217. https://doi.org/10.1007/s11356-013-2313-6
Ribeiro J, de Andrade AR (2006) Investigation of the electrical properties, charging process, and passivation of RuO2–Ta2O5 oxide films. J Electroanal Chem 592:153–162. https://doi.org/10.1016/j.jelechem.2006.05.004
Rocha JHB, Gomes MMS, dos Santos EV, de Moura ECM, da Silva DR, Quiroz MA, Martínez-Huitle CA (2014) Electrochemical degradation of Novacron Yellow C-RG using boron-doped diamond and platinum anodes: direct and indirect oxidation. Electrochim Acta 140:419–426. https://doi.org/10.1016/j.electacta.2014.06.030
Rufino ÉC, Faria LAD, Silva LMD (2011) Influência das condições de resfriamento sobre as propriedades superficiais e eletroquímicas de anodos dimensionalmente estáveis. Química Nova 34(2):200–205. https://doi.org/10.1590/S0100-40422011000200006
Salcedo GM, Kupski L, Degang L, Marube LC, Caldas SS, Primel EG (2019) Determination of fifteen phenols in wastewater from petroleum refinery samples using a dispersive liquid—liquid microextraction and liquid chromatography with a photodiode array detector. Microchem J 146:722–728. https://doi.org/10.1016/j.microc.2019.01.075
Santos TÉ, Silva RS, Eguiluz KIB, Salazar-Banda GR (2015) Development of Ti/(RuO2)0.8(MO2)0.2 (M= Ce, Sn or Ir) anodes for atrazine electro-oxidation. Influence of the synthesis method. Mater Lett 146:4–8. https://doi.org/10.1016/j.matlet.2015.01.145
Santos MO, Santos GOS, Mattedi S, Griza S, Eguiluz KIB, Salazar-Banda GR (2018) Influence of the calcination temperature and ionic liquid used during synthesis procedure on the physical and electrochemical properties of Ti/(RuO2)0.8–(Sb2O4)0.2 anodes. J Electroanal Chem 829:116–128. https://doi.org/10.1016/j.jelechem.2018.10.013
Santos GOS, Silva L, Alves YG, Silva RS, Eguiluz KIB, Salazar-Banda GR (2019) Enhanced stability and electrocatalytic properties of Ti/RuxIr1−xO2 anodes produced by a new laser process. Chem Eng J 355:439–447. https://doi.org/10.1016/j.cej.2018.08.145
Santos G d OS, Vasconcelos VM, da Silva RS, Rodrigo MA, Eguiluz KIB, Salazar-Banda GR (2020a) New laser-based method for the synthesis of stable and active Ti/SnO2–Sb anodes. Electrochim Acta:135478. https://doi.org/10.1016/j.electacta.2019.135478
Santos GOS, Eguiluz KIB, Salazar-Banda GR, Saez C, Rodrigo MA (2020b) Photoelectrolysis of clopyralid wastes with a novel laser-prepared MMO-RuO2TiO2 anode. Chemosphere 244:125455. https://doi.org/10.1016/j.chemosphere.2019.125455
Santos GOS, Dória AR, Vasconcelos VM, Sáez C, Rodrigo MA, Eguiliz KIB, Salazar-Banda GR (2020c) Enhancement of wastewater treatment using novel laser-made Ti/SnO2-Sb anodes with improved electrocatalytic properties. Chemosphere (In press) 259:127475. https://doi.org/10.1016/j.chemosphere.2020.127475
Saxena P, Ruparelia J (2018) Electrochemical degradation of simulated phenolic wastewater using Ti/NixOy-RuO2-SnO2-Sb2O5 anode. Int J Appl Environ Sci 13:811–821
Shao D, Li X, Xu H, Yan W (2014) An improved stable Ti/Sb–SnO2 electrode with high performance in electrochemical oxidation processes. RSC Adv 4:21230–21237. https://doi.org/10.1039/C4RA01990C
Shrivastava P, Moats MS (2009) Wet film application techniques and their effects on the stability of RuO2–TiO2 coated titanium anodes. J Appl Electrochem 39:107–116. https://doi.org/10.1007/s10800-008-9643-y
Sirés I, Brillas E, Oturan MA, Rodrigo MA, Panizza M (2014) Electrochemical advanced oxidation processes: today and tomorrow. A review. Environ Sci Pollut R 21:8336–8367. https://doi.org/10.1007/s11356-014-2783-1
Sopaj F, Rodrigo MA, Oturan N, Podvorica FI, Pinson J, Oturan MA (2015) Influence of the anode materials on the electrochemical oxidation efficiency. Application to oxidative degradation of the pharmaceutical amoxicillin. Chem Eng J 262:286–294. https://doi.org/10.1016/j.cej.2014.09.100
Tchieno FMM, Tonle IK (2018) p-Nitrophenol determination and remediation: an overview. Rev Anal Chem 37. https://doi.org/10.1515/revac-2017-0019
Trellu C, Mousset E, Pechaud Y, Huguenot D, Van Hullebusch ED, Esposito G, Oturan MA (2016) Removal of hydrophobic organic pollutants from soil washing/flushing solutions: a critical review. J Hazard Mater 306:149–174. https://doi.org/10.1016/j.jhazmat.2015.12.008
Wacławek S, Černík M, Dionysiou DD (2020) The development and challenges of oxidative abatement for contaminants of emerging concern. A New Paradigm for Environmental Chemistry and Toxicology:131–152. https://doi.org/10.1007/978-981-13-9447-8_10
Wu W, Huang Z-H, Lim T-T (2014) Recent development of mixed metal oxide anodes for electrochemical oxidation of organic pollutants in water. Appl Catal A-Gen 480:58–78. https://doi.org/10.1016/j.apcata.2014.04.035
Xu LK, Scantlebury JD (2003) Microstructure and electrochemical properties of IrO2-Ta2O5-coated titanium anodes. J Electrochem Soc 150(6):B254–B261
Zhang WM, Ji MW, Wang J (2019) Electrochemical degradation of p-nitrophenol on Cu nanowires and nanocubes. Key Eng Mater 814:76–82. https://doi.org/10.4028/www.scientific.net/KEM.814.76
Zhu X, Ni J (2011) The improvement of boron-doped diamond anode system in electrochemical degradation of p-nitrophenol by zero-valent iron. Electrochim Acta 56:10371–10377. https://doi.org/10.1016/j.electacta.2011.05.062
Acknowledgments
We thank the Núcleo de Estudos Coloidais (NUESC/ITP) for the SEM measurements.
Funding
Financial support from the Brazilian agencies Conselho Nacional de Desenvolvimento Científico e Tecnológico – CNPq (grants 304419/2015-0, 305438/2018-2, 310572/2016-9, 409017/2016-7 and 142034/2020-7), Coordenação de Aperfeiçoamento de Pessoal de Nível Superior – CAPES (88882.365552/2018-01 and 88881.187890/2018-01), and FAPITEC/SE.
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Highlights
• Ti/RuO2–Sb2O4–TiO2 has better properties than Ti/RuO2–Sb2O4, no matter the heating method
• The laser-made Ti/RuO2–Sb2O4–TiO2 has the largest amount of electrocatalytic sites
• The laser-made Ti/RuO2–Sb2O4–TiO2 shows enhanced performance towards 4-NP removal
• The ternary laser-made anode needs low energy to reduce 4-NP by 1 order of magnitude
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Dória, A.R., Santos, G.O.S., Pelegrinelli, M.M.S. et al. Improved 4-nitrophenol removal at Ti/RuO2–Sb2O4–TiO2 laser-made anodes. Environ Sci Pollut Res 28, 23634–23646 (2021). https://doi.org/10.1007/s11356-020-10451-6
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DOI: https://doi.org/10.1007/s11356-020-10451-6