Electrochemical behavior and corrosion resistance of IrO₂-ZrO₂ binary oxide coatings for promoting oxygen evolution in sulfuric acid solution

Abstract

In this study, we prepared Ti/IrO₂-ZrO₂ electrodes with different ZrO₂ contents using zirconium-n-butoxide (C₁₆H₃₆O₄Zr) and chloroiridic acid (H₂IrCl₆) via a sol-gel route. To explore the effect of ZrO₂ content on the surface properties and electrochemical behavior of electrodes, we performed physical characterizations and electrochemical measurements. The obtained results revealed that the binary oxide coating was composed of rutile IrO₂, amorphous ZrO₂, and an IrO₂-ZrO₂ solid solution. The IrO₂-ZrO₂ binary oxide coatings exhibited cracked structures with flat regions. A slight incorporation of ZrO₂ promoted the crystallization of the active component IrO₂. However, the crystallization of IrO₂ was hindered when the added ZrO₂ content was greater than 30at%. The appropriate incorporation of ZrO₂ enhanced the electrocatalytic performance of the pure IrO₂ coating. The Ti/70at%IrO₂-30at%ZrO₂ electrode, with its large active surface area, improved electrocatalytic activity, long service lifetime, and especially, lower cost, is the most effective for promoting oxygen evolution in sulfuric acid solution.

Keywords

electrode / IrO₂-ZrO₂ / oxygen evolution reaction / electrochemical behavior / corrosion resistance

References

[1] Devilliers D, Mahé E. Modified titanium electrodes: Application to Ti/TiO₂/PbO₂ dimensionally stable anodes. Electrochim. Acta, 2010, 55(27): 8207

[2] Zhao Y, YFE Fan LZ, Qiu YF, Yang SH. A new route for the electrodeposition of platinum-nickel alloy nanoparticles on multi-walled carbon nanotubes. Electrochim. Acta, 2007, 52(19): 5873

[3] Lu J L, Lu SF, Wang DL, Yang M, Liu ZL, Xu CW, Jiang SP. Nano-structured Pd_xP_1−x/Ti anodes prepared by electrodeposition for alcohol electrooxidation. Electrochim. Acta, 2009, 54(23): 5486

[4] Fabbri E, Habereder A, Waltar K, Kötz R, Schmidt TJ. Developments and perspectives of oxide-based catalysts for the oxygen evolution reaction. Catal. Sci. Technol., 2014, 4(11): 3800

[5] Siracusano S, Baglio V, Di Blasi A, Briguglio N, Stassi A, Ornelas R, Trifoni E, Antonucci V, Aricò AS. Electrochemical characterization of single cell and short stack PEM electrolyzers based on a nanosized IrO₂ anode electrocatalyst. Int. J. Hydrogen Energy, 2010, 35(11): 5558

[6] Shu J, Qiu ZL, Lv SZ, Zhang KY, Tang DP. Plasmonic enhancement coupling with defect-engineered TiO_2−x: A mode for sensitive photoelectrochemical biosensing. Anal. Chem., 2018, 90(4): 2425

[7] Cai GN, Yu ZZ, Ren RR, Tang DP. Exciton-plasmon interaction between AuNPs/graphene nanohybrids and CdS quantum dots/TiO₂ for photoelectrochemical aptasensing of prostate-specific antigen. ACS Sens., 2018, 3(3): 632

[8] Qiu ZL, Shu J, Tang DP. Near-infrared-to ultraviolet light-mediated photoelectrochemical aptasensing platform for cancer biomarker based on core-shell NaYF₄:Yb, Tm@TiO₂ upconversion microrods. Anal. Chem., 2018, 90(1): 1021

[9] Tang J, Tang DP, Niessner R, Knopp D. A novel strategy for ultra-sensitive electrochemical immunoassay of biomarkers by coupling multifunctional iridium oxide (IrO_x) nanospheres with catalytic recycling of self-produced reactants. Anal. Bioanal. Chem., 2011, 400(7): 2041

[10] Chen XM, Chen GH. Stable Ti/RuO₂-Sb₂O₅-SnO₂ electrodes for O₂ evolution. Electrochim. Acta, 2005, 50(20): 4155

[11] Moradi F, Dehghanian C. Addition of IrO₂ to RuO₂ + TiO₂ coated anodes and its effect on electrochemical performance of anodes in acid media. Prog. Nat. Sci: Mater. Int., 2014, 24(2): 134

[12] Gajić-Krstajić LM, Trišović TL, Krstajić NV. Spectrophotometric study of the anodic corrosion of Ti/RuO₂ electrode in acid sulfate solution. Corros. Sci., 2004, 46(1): 65

[13] Shan R, Zhang ZC, Kan M, Zhang TY, Zan Q, Zhao YX. A novel highly active nanostructured IrO₂/Ti anode for water oxidation. Int. J. Hydrogen Energy, 2015, 40(41): 14279

[14] Vallet CE, Tilak BV, Zuhr RA, Chen CP. Rutherford backscattering spectroscopic study of the failure mechanism of (RuO₂ + TiO₂)/Ti thin film electrodes in H₂SO₄ solutions. J. Electrochem. Soc., 1997, 144(4): 1289

[15] Li BS, Lin A, Gan FX. Preparation and characterization of Ti/IrO₂-Ta₂O₅ anodes for oxygen evolution used to sulfate electrolysis. Rare Met. Mater. Eng., 2007, 36(2): 245

[16] Zhang J J, Hu J M, Zhang J Q, Cao CN. IrO₂-SiO₂ binary oxide films: Geometric or kinetic interpretation of the improved electrocatalytic activity for the oxygen evolution reaction. Int. J. Hydrogen Energy, 2011, 36(9): 5218

[17] Iwakura C, Sakamoto K. Effect of active layer composition on the service life of (SnO₂ and RuO₂)-coated Ti electrodes in sulfuric acid solution. J. Electrochem. Soc., 1985, 132(10): 2420

[18] Pathiraja GC, Nanayakkara N, Wijayasinghe A. Oxygen evolution reaction of Ti/IrO₂-SnO₂ electrodes: a study by cyclic voltammetry. Bull. Mater. Sci., 2016, 39(3): 803

[19] Mazhari HA, Jafarzadeh K, Mirali SM. An investigation of the effect of RuO₂ on the deactivation and corrosion mechanism of a Ti/IrO₂-Ta₂O₅ coating in an OER application. J. Electroanal. Chem., 2016, 777, 67

[20] Vercesi GP, Salamin J Y, Comninellis C. Morphological and microstructural the Ti/IrO₂-Ta₂O₅ electrode: effect of the preparation temperature. Electrochim. Acta, 1991, 36(5–6): 991

[21] Palma-Goyes RE, Vazquez-Arenas J, Ostos C, Torres-Palma RA, González I. The effects of ZrO₂ on the electrocatalysis to yield active chlorine species on Sb₂O₅-doped Ti/RuO₂ anodes. J. Electrochem. Soc, 2016, 163(9): H818

[22] Burke LD, McCarthy M. Oxygen gas evolution at, and deterioration of, RuO₂/ZrO₂-coated titanium anodes at elevated temperature in strong base. Electrochim. Acta, 1984, 29(2): 211

[23] Wang J B, Zhu WP, He XW, Yang SX. Catalytic wet air oxidation of acetic acid over different ruthenium catalysts. Catal. Commun., 2008, 9(13): 2163

[24] Shao YQ, Yi ZY, He C, Zhu J Q, Tang D. Effects of annealing temperature on the structure and capacitive performance of nanoscale Ti/IrO₂-ZrO₂ electrodes. J. Am. Ceram. Soc., 2015, 98(5): 1485

[25] Comninellis CH, Vercesi GP. Characterization of DSA®-type oxygen evolving electrodes: choice of a coating. J. Appl. Electrochem., 1991, 21(4): 335

[26] Terezo AJ, Pereira EC. Preparation and characterisation of Ti/RuO₂ anodes obtained by sol-gel and conventional routes. Mater. Lett., 2002, 53(4–5): 339

[27] Liu B, Wang CY, Chen YQ, Ma BZ, Zhang J L. Effects of calcination temperature on the surface morphology and electrocatalytic properties of Ti/IrO₂-ZrO₂ anodes in an oxygen evolution application. J. Electrochem. Soc., 2018, 165(14): F1192

[28] Malpass GRP, Motheo AJ. Cyclic voltammetric behavior of dimensionally stable anodes in the presence of C1–C3 aldehydes. J. Braz. Chem. Soc., 2003, 14(4): 645

[29] Lee WH, Kim H. Oxidized iridium nanodendrites as catalysts for oxygen evolution reactions. Catal. Commum., 2011, 12(6): 408

[30] Xu W, Haarberg GM, Sunde S, Seland F, Ratvik AP, Zimmerman E, Shimamune T, Gustavsson J, Akre T. Calcination temperature dependent catalytic activity and stability of IrO₂-Ta₂O₅ anodes for oxygen evolution reaction in aqueous sulfate electrolytes. J. Electrochem. Soc, 2017, 164(9): F895

[31] Wu LK, Liu XY, Hu JM. Electrodeposited SiO₂ film: a promising interlayer of a highly active Ti electrode for the oxygen evolution reaction. J. Mater. Chem. A, 2016, 4(30): 11949

[32] Da Silva LA, Alves VA, Da Silva MAP, Trasatti S, Boodts JFC. Morphological chemical and electrochemical properties of Ti/(TiO₂-IrO₂) electrodes. Can. J. Chem., 1997, 75(11): 1483

[33] Pfeifer V, Jones TE, Velasco Vélez JJ, Massué C, Greiner MT, Arrigo R, Teschner D, Girgsdies F, Scherzer M, Allan J, Hashagen M, Weinberg G, Piccinin S, Hävecker M, Knop-Gericke A, Schlögl R. The electronic structure of iridium oxide electrodes active in water splitting. Phys. Chem. Chem. Phys., 2016, 18, 2292

[34] Xu RD, Huang LP, Zhou JF, Zhan P, Guan YY, Kong Y. Effects of tungsten carbide on electrochemical properties and microstructural features of Al/Pb-PANI-WC composite inert anodes used in zinc electrowinning. Hydrometallurgy, 2012, 125–126, 8

[35] Audichon T, Morisset S, Napporn TW, Kokoh KB, Comminges C, Morals C. Effect of adding CeO₂ to RuO₂-IrO₂ mixed nanocatalysts: activity towards the oxygen evolution reaction and stability in acidic media. ChemElectroChem, 2015, 2(8): 1128

[36] Rasten E, Hagen G, Tunold R. Electrocatalysts in water electrolysis with solid polymer electrolyte. Electrochim. Acta, 2003, 48(25–26): 3945

[37] Santana MHP, De Faria LA, Boodts JFC. Effect of preparation procedure of IrO₂-Nb₂O₅ anodes on surface and electrocatalytic properties. J. Appl. Electrochem., 2005, 35(9): 915

[38] Da Silva LM, De Faria LA, Boodts JFC. Electrochemical ozone production: influence of the supporting electrolyte on kinetics and current efficiency. Electrochim. Acta, 2003, 48(6): 699

[39] Lassali TAF, Boodts JFC, Bulhoes LOS. Charging processes and electrocatalytic properties of IrO₂/TiO₂/SnO₂ oxide films investigated by in situ AC impedance measurements. Electrochim. Acta, 1999, 44(24): 4203

[40] Hu J M, Meng HM, Zhang JQ, Cao CN. Degradation mechanism of long service life Ti/IrO₂-Ta₂O₅ oxide anodes in sulphuric acid. Corros. Sci., 2002, 44(8): 1655

[41] Hou YY, Hu JM, Liu L, Zhang JQ, Cao CN. Effects of calcination temperature on electrocatalytic activities of Ti/IrO₂ electrodes in methanol aqueous solutions. Electrochim. Acta, 2006, 51(28): 6258

[42] Palmas S, Polcaro AM, Ferrara F, Ruiz JR, Delogu F, Bonatto-Minella C, Mulas G. Electrochemical performance of mechanically treated SnO₂ powers for OER in acid solution. J. Appl. Electrochem., 2008, 38(7): 907

[43] Piela B, Wrona PK. Capacitance of the gold electrode in 0.5 M H₂SO₄ solution: a.c. impedance studies. J. Appl. Electroanal. Chem., 1995, 388(1–2): 69

[44] Yang HT, Liu HR, Guo ZC, Chen BM, Zhang YC, Huang H, Li XL, Fu RC, Xu RD. Electrochemical behavior of rolled Pb-0.8%Ag anodes. Hydrometallurgy, 2013, 140, 144

[45] Alves VA, da Silva LA, Boodts JFC. Surface characterisation of IrO₂/TiO₂/CeO₂ oxide electrodes and Faradaic impedance investigation of the oxygen evolution reaction from alkaline solution. Electrochim. Acta, 1998, 44(8–9): 1525

[46] Ye ZG, Meng HM, Sun DB. New degradation mechanism of Ti/IrO₂-MnO₂ anode for oxygen evolution in 0.5 M H₂SO₄ solution. Electrochim. Acta, 2008, 53(18): 5639

[47] Martelli GN, Ornelas R, Faita G. Deactivation mechanisms of oxygen evolving anodes at high current densities. Electrochim. Acta, 1994, 39(11–12): 1551

[48] Kötz R, Neff H, Stucki S. Anodic iridium oxide films: XPS-studies of oxidation state changes and O₂-evolution. J. Electrochem. Soc., 1984, 131(1): 72

[49] Song Y, Wei G, Xiong R. Structure and properties of PbO₂-CeO₂ anodes on stainless steel. Electrochim. Acta, 2007, 52(24): 7022

[50] Yang HT, Chen BM, Liu HR, Guo ZC, Zhang YC, Li XL, Xu RD. Effects of manganese nitrate concentration on the performance of an aluminum substrate β-PbO₂-MnO₂-WC-ZrO₂ composite electrode material. Int. J. Hydrogen Energy, 2014, 39(7): 3087

[51] Zhang W, Ghali E, Houlachi G. Review of oxide coated catalytic titanium anodes performance for metal electrowinning. Hydrometallurgy, 2017, 169, 456