Abstract
In this study, linear polarization resistance (LPR) of pulse reverse electrodeposited graphene oxide (PREGO) coating is optimized by design of experiments approach (central composite design). Pulse current density (i), cathodic (T c) and anodic (T a) pulse durations, and total electrodeposition time (T t) are selected as the substantial factors. The best prediction model proposes a definitive linear relation without any significant interaction of the LPR by analysis of variance. The desirable value of LPR was predicted equal to 5358 Ω cm2, obtaining at the pulse current density of 235.62 mA cm−2, T a of 7.75 ms, T c equal to 3.25 ms (f = 100 Hz), and T t of approximately 225 s. Appearance of the XRD peaks at 25.11° and 27.18° and declining coating impedance up to 21 Ω cm2, as well as the elimination of functional groups at FT-IR spectra, are vividly promised the formation of sp2 domains in the PREGO coating.
This is a preview of subscription content, access via your institution.








References
Zhu Y, Murali S, Cai W, Li X, Suk J, Potts JR, Ruoff RS (2010) Graphene and graphene oxide: synthesis, production, and applications. Adv Mater 22:3906–3924
Shao Y, Wang J, Wu H, Liu J, Aksay IA, Lin Y (2010) Graphene based electrochemical sensors and biosensors: a review. Electroanal 22:1027–1036
Jagannadham K (2012) Thermal conductivity of copper-graphene composite films synthesized by electrochemical deposition with exfoliated graphene platelets. Metall Mater Trans B 43B:316–324
Jo I, Hsu I, Lee YJ, Sadeghi M, Kim S, Cronin S, Tutuc E, Banerjee SK, Yao Z, Shi L (2011) Low-frequency acoustic phonon temperature distribution in electrically biased graphene. Nano Lett 11:85–90
Frank IW, Tanenbaum DM, Zande AM, McEuen PL (2007) Mechanical properties of suspended graphene sheets. Vac Sci Tech 25:2558–2562
Poetschke M, Rocha CG, Foa Torres LEF, Roche S, Cuniberti G (2010) Modeling graphene-based nanoelectromechanical devices. Phys Rev B 81:193401–193404
Singh Raman RK, Banerjee PC, Lobo DE, Gullapalli H, Sumandasa M, Kumar A, Choudhary L, Tkacz R, Ajayan PM, Majumder M (2012) Protecting copper from electrochemical degradation by graphene coating. Carbon 50:4040–4045
Kirkland NT, Schiller T, Medhekar N, Birbilis N (2012) Exploring graphene as a corrosion protection barrier. Corros Sci 56:1–4
Yi Lih ET, Mat Zaid R, Ling Ling T, Feng Chong K (2012) Facile corrosion protection coating from graphene. Int J Chem Eng Appl 3:453–455
Singh BP, Nayak S, Nanda KK, Jena BK, Bhattacharjee S, Besra L (2013) The production of a corrosion resistant graphene reinforced composite coating on copper by electrophoretic deposition. Carbon 61:47–56
Kousalya AS, Kumar A, Paul R, Zemlyanov D, Fisher TS (2013) Graphene: an effective oxidation barrier coating for liquid and two-phase cooling systems. Corros Sci 69:5–10
Sahu SC, Samantara AK, Seth M, Parwaiz S, Singh BP, Rath PC, Jena BK (2013) A facile electrochemical approach for development of highly corrosion protective coatings using graphene nanosheets. Electrochem Commun 32:22–26
Praveen Kumar CM, Venkatesha TV, Shabadi R (2013) Preparation and corrosion behavior of Ni and Ni-graphene composite coatings. Mater Res Bull 48:1477–1483
Singh BP, Jena BK, Bhattacharjee S, Besra L (2013) Development of oxidation and corrosion resistance hydrophobic graphene oxide-polymer composite coating on copper. Surf Coat Tech 232:475–481
Nayak PK, Hsu C, Wang S, Sung JC, Huang J (2013) Graphene coated Ni films: a protective coating. Thin Solid Films 529:312–316
Chen S, Brown L, Levendorf M, Cai W, Ju S, Edgeworth J, Li X, Magnuson C, Velamakanni A, Piner RD, Kang J, Park J, Ruoff RS (2011) Oxidation resistance of graphene-coated Cu and Cu/Ni alloy. ACS Nano 5:1321–1327
Dennis RV, Viyannalage LT, Gaikwad AV, Rout TK, Banerjee S (2013) Graphene nanocomposite coatings for protecting low-alloy steels from corrosion. Am Ceram Soc Bull 92:18–24
Ci L, Song L, Jariwala D, Elias AL, Gao W, Weies M, Ajayan P (2009) Graphene shape control by multistage cutting and transfer. Adv Mater 21:1–5
Zhao J, Chen G, Zhang W, Li P, Wang L, Yue Q, Wang H, Dong R, Yan X, Liu J (2011) High-resolution separation of graphene oxide by capillary electrophoresis. Anal Chem 83:9100–9106
Vadahanambi S, Jung J, Oh I (2011) Microwave syntheses of graphene and graphene decorated with metal nanoparticles. Carbon 49:4449–4457
Guo HL, Wang XF, Qian QY, Wang FB, Xia XH (2009) A green approach to the synthesis of graphene nanosheets. ACS Nano 3:2653–2659
Peng X, Liu X, Diamond D, Lau KT (2011) Synthesis of electrochemically-reduced graphene oxide film with controllable size and thickness and its use in supercapacitor. Carbon 49:3488–3496
Chen L, Tang Y, Wang K, Liu C, Luo S (2011) Direct electrodeposition of reduced graphene oxide on glassy carbon electrode and its electrochemical application. Electrochem Commun 13:133–137
Harima Y, Setodoi S, Imae I, Komaguchi K, Ooyama Y, Ohshita J, Mizota H, Yano J (2011) Electrochemical reduction of graphene oxide in organic solvents. Electrochim Acta 56:5363–5368
Yaghoubinezhad Y, Afshar A (2015) Design of experiments for pulse reverse electrodeposition of graphene oxide towards hydrogen evolution reaction. ECS J Solid State Sci Technol 4:M7–M17
Hilder M, Winther-Jensen B, Li D, Forsyth M, MacFarlane DR (2011) Direct electro-deposition of graphene from aqueous suspensions. Phys Chem Chem Phys 13:9187–9193
Ye W, Zhang X, Chen Y, Du Y, Zhou F, Wang C (2013) Pulsed electrodeposition of reduced graphene oxide on glass carbon electrode as an effective support of electrodeposited Pt microspherical particles: nucleation studies and the application for methanol electro-oxidation. Int J Electrochem Sci 8:2122–2139
Tsutakawa RK (1972) Design of experiment for bioassay. J Am Stat Assoc 67:584–590
Nsengiyumva C, Beer JOD, Wauw WV, Vlietinck AJ, Parmentier F (1997) An exprimental design approach to selecting the optimum liquid chromatographic conditions for the determination of vitamins B1, B2-phosphate, B3, B6 and C in effervescent tablets containing saccharin and sunset yellow FCF. Chromatographia 44:634–644
Yi BJ, Chung GB, Na HY, Kim WK, Suh IH (2003) Design and experiment of a 3-DOF parallel micromechanism utilizing flexure hinges. Robot Auton Trans B 19:604–612
Man HL, Behera SK, Park HS (2010) Optimization of operational parameters for ethanol production from Korean food waste leachate. Int J Environ Sci Tech 7(1):157–164
Poroch-Seritan M, Gutt S, Gutt G, Cretescu I, Cojocaru C, Severin T (2011) Design of experiments for statistical modeling and multi-response optimization of nickel electroplating process. Chem Eng Res Des 89:136–147
Ravikumar K, Pakshirajan K, Swaminathan T, Balu K (2005) Optimization of batch process parameters using response surface methodology for dye removal by a novel adsorbent. Chem Eng J 105:131–138
Wang JP, Chen YZ, Ge XW, Yu HQ (2007) Optimization of coagulation–flocculation process for a paper-recycling wastewater treatment using response surface methodology. Colloid Surf A 302:204–210
Aleboyeh A, Daneshvar N, Kasiri MB (2008) Optimization of C.I. Acid Red 14 azo dye removal by electrocoagulation batch process with response surface methodology. Chem Eng Process 47:827–832
Chen X, Wang W, Li S, Xue J, Fan L, Sheng Z, Chen Y (2010) Optimization of ultrasound-assisted extraction of lingzhi polysaccharides using response surface methodology and its inhibitory effect on cervical cancer cells. Carbohydr Polym 80:944–948
Imanieh I, Yousefi E, Dolati A, Mohammadi MR (2013) Experiments design for hardness optimization of the Ni-Cr alloy electrodeposited by pulse plating. Acta Metall Sin 26:558–564
Ahmadi M, Vahabzadeh F, Bonakdarpour B, Mofarrah E, Mehranian M (2005) Application of the central composite design and response surface methodology to the advanced treatment of olive oil processing wastewater using Fenton’s peroxidation. J Hazard Mater 123:187–195
Rosa PAJ, Azevedo AM, Aires Barros MR (2007) Application of central composite design to the optimisation of aqueous two-phase extraction of human antibodies. J Chromatogr A 1141:50–60
Hummers WS, Offeman RE (1958) Preparation of graphene oxide. J Am Chem Soc 80:1339
Chandrasekar MS, Pushpavanam M (2008) Pulse and pulse reverse plating-conceptual, advantages and applications. Electrochim Acta 53:3313–3322
Zhang Y, Yang Y, Xiao P, Zhang X, Lu L, Li L (2009) Preparation of Ni nanoparticle-TiO2 nanotube composite by pulse electrodeposition. Mater Lett 63:2429–2431
Xiao F, Xu Y (2012) Pulse electrodeposition of manganese oxide for high-rate capability supercapacitors. Int J Electrochem Sci 7:7440–7450
Low CTJ, Walsh FC, Chakrabarti MH, Hashim MA (2013) Electrochemical approaches to the production of graphene flakes and their potential applications. Carbon 54:1–21
Kauppila J, Kunnasa P, Damlina P, Viinikanoja A, Kvarnström C (2013) Electrochemical reduction of graphene oxide films in aqueous and organic solutions. Electrochim Acta 89:84–89
Cote LJ, Kim J, Tung VC, Luo J, Kim F, Huang J (2011) Graphene oxide as surfactant sheets. Pure Appl Chem 83:95–110
Antony J (2003) Design of experiments for engineers and scientists. Elsevier Science & Technology Books, New York
Khorasani S, Motieifar A, Rashidian B (2003) Optimal pulse shapes for reperiodic reverse electroplating. Iran J Sci Technol 27:701–711
Yang D, Velamakanni A, Bozoklu G, Park S, Stoller M, Piner RD, Stankovich S, Jung I, Field DA, Ventrice CA Jr, Ruoff RS (2009) Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and micro-Raman spectroscopy. Carbon 47:145–152
Ramesha GK, Sampath S (2009) Electrochemical reduction of oriented graphene oxide films: an in situ Raman spectroelectrochemical study. J Phys Chem Lett 113:7985–7989
Paredes I, Villar Rodil S, Alonso M, Tascon JMD (2008) Graphene oxide dispersions in organic solvent. Langmuir 24:10560–10564
Peng X, Liu X, Diamond D, Tong Lau K (2011) Synthesis of electrochemically-reduced graphene oxide film with controllable size and thickness and its use in supercapacitor. Carbon 49:3488–3496
Park S, Ruoff RS (2009) Chemical methods for the production of graphenes. Nat Nanotechnol 58:1–8
Peng XY, Liu XX, Diamond D, Tong Lau K (2011) Synthesis of electrochemically-reduced graphene oxide film with controllable size and thickness and its use in supercapacitor. Carbon 49:3488–3496
Grinou A, Yun Y, Cho S, Park H, Jin H (2012) Dispersion of Pt nanoparticle-doped reduced graphene oxide using aniline as a stabilizer. Materials 5:2927–2936
Vázquez-Gómez L, Cattarin S, Guerriero P, Musiani M (2008) Hydrogen evolution on porous Ni cathodes modified by spontaneous deposition of Ru or Ir. Electrochim Acta 53:8310–8318
Becerril HA, Mao J, Liu Z, Stoltenberg RM, Bao Z, Chen Y (2008) Evaluation of solution-processed reduced graphene oxide films as transparent conductors. ACS Nano 2:463–470
Fei C, Xiaoli Z (2012) A method based on electrodeposition of reduced graphene oxide on glassy carbon electrode for sensitive detection of theophylline. J Solid State Electrochem 12:1867–1864
Acknowledgments
We would like to thank the Iran Nanotechnology Initiative Council for the partial financial support of the work.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Yaghoubinezhad, Y., Afshar, A. Experimental design for optimizing the corrosion resistance of pulse reverse electrodeposited graphene oxide thin film. J Solid State Electrochem 19, 1367–1380 (2015). https://doi.org/10.1007/s10008-015-2754-6
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10008-015-2754-6