Based on the hypothesis that the electrodeposition conditions may have effects on the developed electrode’s oxidation performance, the present study aimed at investigating the effects of a graphite/PbO2 anode preparation conditions (current intensity, Pb(NO3)2 concentration, HNO3 concentration, and temperature) on leachate treatment efficiency. Synthesis conditions were varied to improve the performance of the electrode, and leachate treatment efficiencies were evaluated using anodes prepared at different conditions. The Box–Behnken design was used as an experimental design for achieving the goal. The effect of variables on the system’s outcome was modeled by response surface methodology and artificial neural network. The variation in chemical oxygen demand (COD) removal efficiency from 7.81 to 24.58% for 2 h of electrolysis demonstrates significant influences of anode preparation conditions on its performance. The optimum conditions were attained as 0.64 A of current intensity, 0.16 mol L−1 of Pb(NO3)2, 0.16 mol L−1 of HNO3, and 76.98 °C of temperature. The PbO2 electrode developed at optimum conditions yielded 79 ± 1.7% COD removal efficiency of leachate at 8 h. The study results show that electrode synthesis conditions affect the oxidation ability of the electrode, and optimization of the same can significantly improve the treatment performance.
This is a preview of subscription content, log in to check access.
Buy single article
Instant access to the full article PDF.
Price includes VAT for USA
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
This is the net price. Taxes to be calculated in checkout.
Abaci S, Pekmez K, Hokelek T, Yildiz A (2000) Investigation of some parameters influencing electrocrystallisation of PbO2. J Power Sources 88:232–236
Abaci S, Tamer U, Pekmez K, Yildiz A (2005) Performance of different crystal structures of PbO2 on electrochemical degradation of phenol in aqueous solution. Appl Surf Sci 240:112–119
An H, Li Q, Tao D, Cui H, Xu X, Ding L, Sun L, Zhai J (2011) The synthesis and characterization of Ti/SnO2–Sb2O3/PbO2 electrodes: the influence of morphology caused by different electrochemical deposition time. Appl Surf Sci 258:218–224
Anglada A, Urtiaga A, Ortiz I, Mantzavinos D, Diamadopoulos E (2010) Boron-doped diamond anodic treatment of landfill leachate: evaluation of operating variables and formation of oxidation. Water Res 5:828–838
Bashir MJK, Isa MH, Kutty SRM, Awang ZB, Aziz HA, Mohajeri S, Farooqi IH (2009) Landfill leachate treatment by electrochemical oxidation. Waste Manage 29:2534–2541
Bicelli LP, Bozzini B, Mele C, D’Urzo L (2008) A review of nanostructural aspects of metal electrodeposition. Int J Electrochem Sci 3:356–408
Campbell SA, Peter LM (1988) A study of the effect of deposition current density on the structure of electrodeposited α-PbO2. Electrochim Acta 34:943–949
Candioti LV, De Zan MM, Cámara MS, Goicoechea HC (2014) Experimental design and multiple response optimization. Using the desirability function in analytical methods development. Talanta 124:123–138
Carr JP, Hampson NA (1972) The lead dioxide electrode. Chem Rev 72:679–703
Chiang LC, Chang JE, Wen TC (1995) Electrochemical treatability of refractory pollutants in landfill leachate. Hazard Waste Hazard Mater 12(1):71–82
Chiang LC, Chang JE, Chung CT (2001) Electrochemical oxidation combined with physical-chemical pretreatment processes for the treatment of refractory landfill leachate. Environ Eng Sci 18(6):369–379
Dai Q, Xia Y, Chen J (2016) Mechanism of enhanced electrochemical degradation of highly concentrated aspirin wastewater using a rare earth La–Y co-doped PbO2 electrode. Electrochim Acta 188:871–881
Duan Y, Wen Q, Chen Y, Duan T, Zhou Y (2014) Preparation and characterization of TiN-doped Ti/SnO2–Sb electrode by dip coating for orange II decolorization. Appl Surf Sci 320:746–755
Duan X, Zhao C, Liu W, Zhao X, Chang L (2017) Fabrication of a novel PbO2 electrode with a graphene nanosheet interlayer for electrochemical oxidation of 2-chlorophenol. Electrochim Acta 240:424–436
Fernandes A, Pacheco MJ, Ciríaco L, Lopes A (2015) Review on the electrochemical processes for the treatment of sanitary landfill leachates: present and future. Appl. Catal. B Environ. 176–177:183–200
Garson GD (1991) Interpreting neural-network connection weights. AI Expert 6:47–51
Ghasemi S, Fazllolah M, Shamsipur M (2007) Electrochemical deposition of lead dioxide in the presence of polyvinylpyrrolidone A morphological study. Electrochim Acta 53:459–467
Hamdy A, Mostafa MK, Nasr M (2019) Regression analysis and artificial intelligence for removal of methylene blue from aqueous solutions using nanoscale zero-valent iron. Int J Environ Sci Technol 16:357–372
Holzwarth U, Gibson N (2011) The Scherrer equation versus the ‘Debye–Scherrer equation’. Nat Nanotechnol 6:534
Ihara I, Kanamura K, Shimada E, Watanabe T (2004) High gradient magnetic separation combined with electrocoagulation and electrochemical oxidation for the treatment of landfill leachate. IEEE Trans Appl Superconduct 14(2):1558–1560
Kapoor A, Yang RT (1989) Correlation of equilibrium adsorption data of condensible vapours on porous adsorbents. Gas Sep Purif 3:187–192
Karri RR, Tanzifi M, Yaraki MT, Sahu JN (2018) Optimization and modeling of methyl orange adsorption onto polyaniline nano-adsorbent through response surface methodology and differential evolution embedded neural network. J Environ Manage 223:517–529
Kundu P, Paul V, Kumar V, Mishra IM (2015) Formulation development, modeling and optimization of emulsification process using evolving RSM coupled hybrid ANN-GA framework. Chem Eng Res Des 4:773–790
Leitner V, Malucelli LC, Pincerati MR, Maranho LT (2019) Rhizospheric bacteria with potential to degrade landfill leachate. Int J Environ Sci Technol 16:1581–1588
Li X, Pletcher D, Walsh FC (2009) A novel flow battery: a lead acid battery based on an electrolyte with soluble lead(II) Part VII. Further studies of the lead dioxide positive electrode. Electrochim Acta 54:4688–4695
Li J, Yang Z, Xu H, Song P, Huang J, Xu R, Zhang Y, Zhou Y (2016) Electrochemical treatment of mature landfill leachate using Ti/RuO2–IrO2 and Al electrode: optimization and mechanism. RSC Adv. 6:47509–47519
Li X, Xu H, Yan W (2017) Effects of twelve sodium dodecyl sulfate (SDS) on electro-catalytic performance and stability of PbO2 electrode. J Alloy Compd 718:386–395
Low CTJ, Pletcher D, Walsh FC (2009) The electrodeposition of highly reflective lead dioxide coatings. Electrochem Commun 11:1301–1304
Mandal P, Dubey BK, Gupta AK (2017) Review on landfill leachate treatment by electrochemical oxidation: drawbacks, challenges and future scope. Waste Manage 69:250–273
Mandal P, Gupta AK, Dubey BK (2018) A novel approach towards multivariate optimization of graphite/PbO2 anode synthesis conditions: insight into its enhanced oxidation ability and physicochemical characteristics. J Environ Chem Eng 6:4438–4451
Montgomery DC (2013) Design and analysis of experiments, 8th edn. Wiley, Delhi
Mukherjee DS, Rajanikanth BS (2019) Prediction of variation of oxides of nitrogen in plasma-based diesel exhaust treatment using artificial neural network. Int J Environ Sci Technol. https://doi.org/10.1007/s13762-019-02242-5
Munichandraiah N (1992) Physicochemical properties of electrodeposited β-lead dioxide: effect of deposition current density. J Appl Electrochem 22:825–829
Panizza M, Delucchi M, Sirés I (2010) Electrochemical process for the treatment of landfill leachate. J Appl Electrochem 40(10):1721–1727
Renou S, Givaudan JG, Poulain S, Dirassouyan F, Moulin P (2008) Landfill leachate treatment: review and opportunity. J Hazard Mater 150(3):468–493
Saravanathamizhan R, Vardhan KH, Prakash DG (2015) RSM and ANN modeling for electro-oxidation of simulated wastewater using CSTER. Desalin Water Treat 3994:1–8
Scherrer P (1918) Bestimmung der Grosse und der Inneren Struktur von Kolloidteilchen Mittels Rontgenstrahlen, Nachrichten von der Gesellschaft der Wissenschaften zu Gottingen. Math Phys Klasse 2:98–100
Shen KP, Wei LX (2003) Morphologic study of electrochemically formed lead dioxide. Electrochim Acta 48:1743–1747
Silveira JE, Zazo JA, Pliego G, Bidóia ED, Moraes PB (2015) Electrochemical oxidation of landfill leachate in a flow reactor: optimization using response surface methodology. Environ Sci Pollut Res 22:5831–5841
Silveira JE, Claro EMT, Paz WS, Oliveira AS, Zazo JA, Casas JA (2018) Optimization of disperse blue 3 mineralization by UV-LED/FeTiO3 activated persulfate using response surface methodology. J Taiwan Inst Chem Eng 85:66–73
Sirés I, Low CTJ, Ponce-de-León C, Walsh FC (2010) The characterisation of PbO2-coated electrodes prepared from aqueous methanesulfonic acid under controlled deposition conditions. Electrochim Acta 55:2163–2172
Sizirici B, Yildiz I (2017) Adsorption capacity of iron oxide-coated gravel for landfill leachate: simultaneous study. Int J Environ Sci Technol 14:1027–1036
Thanos JCG, Wabner DW (1985) Structural changes of the texture of β-lead dioxide-titanium anodes during the oxygen/ozone electrosynthesis in neutral and acidic electrolytes. J Electroanal Chem 182:37–49
Velichenko AB, Amadelli R, Benedetti A, Girenko DV, Kovalyov SV, Danilov FI (2002) Electrosynthesis and physicochemical properties of PbO2 films. J Electrochem Soc 149:445–449
Velichenko AB, Amadelli R, Gruzdeva EV, Luk’yanenko TV, Danilov FI (2009) Electrodeposition of lead dioxide from methanesulfonate solutions. J Power Sources 191:103–110
Viana DF, Salazar-banda GR, Leite MS (2018) Electrochemical degradation of reactive black 5 with surface response and artificial neural networks optimization models. Sep Sci Technol 53(16):2647–2661
Willmott CJ, Matsuura K (2005) Advantages of the mean absolute error (MAE) over the root mean square error (RMSE) in assessing average model performance. Clim Res 30:79–82
Xu M, Mao Y, Song W, Ouyang X, Hu Y, Wei Y (2018) Preparation and characterization of Fe–Ce co-doped Ti/TiO2 NTs/PbO2 nanocomposite electrodes for efficient electrocatalytic degradation of organic pollutants. J Electroanal Chem 823:193–202
Xue J, Yu L, Li G (2017) Influence of molecular structure of imidazolium based ionic liquids on the electrochemical oxidation performances of resulting PbO2 deposits. Int J Electrochem Sci 12:4795–4810
Yeh CJ, Lo SL, Kuo J, Chou YC (2018) Optimization of landfill leachate treatment by microwave oxidation using the Taguchi method. Int J Environ Sci Technol 15:2075–2086
Zhang H, Li Y, Wu X, Zhang Y, Zhang D (2010) Application of response surface methodology to the treatment landfill leachate in a three-dimensional electrochemical reactor. Waste Manage 30:2096–2102
Zhang H, Ran X, Wu X, Zhang D (2011) Evaluation of electro-oxidation of biologically treated landfill leachate using response surface methodology. J Hazard Mater 188:261–268
Zhao W, Xing J, Chen D, Jin D, Shen J (2016) Electrochemical degradation of Musk ketone in aqueous solutions using a novel porous Ti/SnO2–Sb2O3/PbO2 electrodes. J Electroanal Chem 775:179–188
The authors are very much thankful to Indian Institute of Technology Kharagpur, for providing infrastructural facilities for this study.
Conflict of interest
The authors declare that there is no conflict of interest. Joint Committee on Powder Diffraction Standards (JCPDS) cards of International Centre for Diffraction Data (ICDD) database 2017 was used in the study.
Editorial responsibility: Fatih Şen.
Electronic supplementary material
Below is the link to the electronic supplementary material.
About this article
Cite this article
Mandal, P., Gupta, A.K. & Dubey, B.K. Synthesis of graphite/PbO2 anode: electrodeposition process modeling for improved landfill leachate treatment using RSM and ANN approach. Int. J. Environ. Sci. Technol. 17, 1947–1962 (2020). https://doi.org/10.1007/s13762-019-02460-x
- Lead dioxide anode
- Response surface methodology
- Artificial neural network
- Electrochemical oxidation