Abstract
This study introduces a new surface-renewable electrode based on a sol–gel derived graphene ceramic composite. The electrode was prepared by dispersing graphene nanosheets into a solution of the sol–gel precursors containing methyl triethoxysilane in methanol and hydrochloric acid. During hydrolysis of methyl triethoxysilane, the graphene nanosheets are trapped in the gel. After moulding and drying the composite, it can be used as a surface-renewable electrode to which we refer as a graphene ceramic composite electrode (GCCE). Cyclic voltammograms of the hexacyanoferrate(II/III) model redox system at the GCCE were compared to those obtained with a conventional carbon ceramic electrode and showed a highly improved electron transfer rate at the GCCE. The electrocatalytic oxidation of ascorbic acid as a model analyte was then studied at working potential of 50 mV and over the 3–84 μM concentration range. It revealed a sensitivity of 6.06 μA μM−1 cm−2 and a detection limit of 0.82 μM. The GCCE was successfully applied to the determination of ascorbic acid in orange juice and urine samples. Advantages such as good mechanical and chemical stability, ease of fabrication, and reproducible preparation make the GCCE a potentially useful and widely applicable renewable electrode for use in routine analysis.
Similar content being viewed by others
References
Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV, Grigorieva IV, Firsov AA (2004) Electric field effect in atomically thin carbon films. Science 306(5696):666–669. doi:10.1126/science.1102896
Geim AK, Novoselov KS (2010) The rise of graphene. Nat Mater 6:183–191. doi:10.1038/nmat1849
Choi W, Lahiri I, Seelaboyina R, Kang YS (2010) Synthesis of graphene and its applications. Crit Rev Solid State Mater Sci 35(1):52–71
Kuila T, Bose S, Khanra P, Mishra AK, Kim NH, Lee JH (2011) Recent advances in graphene-based biosensors. Biosens Bioelectron 26(12):4637–4648. doi:10.1016/j.bios.2011.05.039
Allen MJ, Tung VC, Kaner RB (2010) Honeycomb carbon: a review of graphene. Chem Rev 110(1):132–145. doi:10.1021/cr900070d
Gan T, Hu S (2011) Electrochemical sensors based on graphene materials. Microchim Acta 175(1):1–19. doi:10.1007/s00604-011-0639-7
Briza PL, Merkoci A (2012) Carbon nanotubes and graphene in analytical sciences. Microchim Acta 179(1):1–16. doi:10.1007/s00604-012-0871-9
Li F, Li J, Feng Y, Yang L, Du Z (2011) Electrochemical behavior of graphene doped carbon paste electrode and its application for sensitive determination of ascorbic. Sensors Actuators B 157(1):110–114. doi:10.1016/j.snb.2011.03.033
Parvin MH (2011) Graphene paste electrode for detection of chlorpromazine. Electrochem Commun 13(4):366–369. doi:10.1016/j.elecom.2011.01.027
Tsionsky M, Gun G, Glezer V, Lev O (1994) Sol–gel-derived ceramic-carbon composite electrodes: introduction and scope of applications. Anal Chem 66(10):1747–1753. doi:10.1021/ac00082a024
Salimi A, Roushani M (2005) Non-enzymatic glucose detection free of ascorbic acid interference using nickel powder and nafion sol–gel dispersed renewable carbon ceramic electrode. Electrochem Commun 7(9):879–887. doi:10.1016/j.elecom.2005.05.009
Lei CX, Hu SQ, Gao N, Shen GL, Yu RQ (2004) An amperometric hydrogen peroxide biosensor based on immobilizing horseradish peroxidase to a nano-Au monolayer supported by sol–gel derived carbon ceramic electrode. Bioelectrochemistry 65(1):33–39. doi:10.1016/j.bioelechem.2004.06.002
Li Y, Kuan CF, Chen CH, Kuan HC, Yip MC, Chiu SL, Chiang CL (2012) Preparation, thermal stability and electrical properties of PMMA/functionalized graphene oxide nanosheets composites. Mater Chem Phys 134(2–3):677–685. doi:10.1016/j.matchemphys.2012.03.050
Xu Y, Bai H, Lu G, Li C, Shi G (2008) Flexible graphene films via the filtration of water-soluble noncovalent functionalized graphene sheets. J Am Chem Soc 130(18):5856–5857. doi:10.1021/ja800745y
Stankovich S, Dikin DA, Piner RD, Kohlhaas KA, Kleinhammes A, Jia Y, Wu Y, Nguyen ST, Ruoff RS (2007) Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45(7):1558–1565. doi:10.1016/j.carbon.2007.02.034
Razmi H, Mohammad-Rezaei R (2011) Preparation of tungsten oxide nanoporous thin film at carbon ceramic electrode for electrocatalytic applications. Electrochim Acta 56(20):7220–7223. doi:10.1016/j.electacta.2011.04.018
Zhang K, Zhang LL, Zhao XS, Wu JS (2010) Graphene/polyaniline nanofiber composites as supercapacitor electrodes. Chem Mater 22(4):1392–1401. doi:10.1021/cm902876u
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(2):133–137. doi:10.1016/j.elecom.2010.11.033
Henstridge MC, Laborda E, Dickinson EJF, Compton RG (2012) Redox systems obeying Marcus-Hush-Chidsey electrode kinetics do not obey the Randles-Sevcik equation for linear sweep voltammetry. J Electroanal Chem 664:73–79
Gai P, Zhang H, Zhang Y, Liu W, Zhu G, Zhang X, Chen J (2013) Simultaneous electrochemical detection of ascorbic acid, dopamine and uric acid based on nitrogen doped porous carbon nanopolyhedra. J Mater Chem B 1(21):2742–2749. doi:10.1039/C3TB20215A
Sun CL, Lee HH, Yang JM, Wu CC (2011) The simultaneous electrochemical detection of ascorbic acid, dopamine, and uric acid using graphene/size-selected Pt nanocomposites. Biosens Bioelectron 26(8):3450–3455. doi:10.1016/j.bios.2011.01.023
Hutton EA, Pauliukaite R, Hocevar SB, Ogorevc B, Smyth MR (2010) Amperometric microsensor for direct probing of ascorbic acid in human gastric juice. Anal Chim Acta 678(2):176–182. doi:10.1016/j.aca.2010.08.027
Xi L, Ren D, Luo J, Zhu Y (2010) Electrochemical analysis of ascorbic acid using copper nanoparticles/Polyaniline modified glassy carbon electrode. J Electroanal Chem 650(1):127–134. doi:10.1016/j.jelechem.2010.08.014
Weng CJ, Chen YL, Chien CM, Hsu SC, Jhuo YS, Yeh JM, Dai CF (2013) Preparation of gold decorated SiO2@polyaniline core-shell microspheres and application as a sensor for ascorbic acid. Electrochim Acta 95:162–169. doi:10.1016/j.electacta.2013.01.150
Wu GH, Wu YF, Liu XW, Rong MC, Chen XM, Chen X (2012) An electrochemical ascorbic acid sensor based on palladium nanoparticles supported on graphene oxide. Anal Chim Acta 745:33–37. doi:10.1016/j.aca.2012.07.034
Yang L, Liu S, Zhang Q, Li F (2012) Simultaneous electrochemical determination of dopamine and ascorbic acid, using AuNPs@polyaniline core-shell nanocomposites modified electrode. Talanta 89:136–141. doi:10.1016/j.talanta.2011.12.002
Acknowledgments
The authors gratefully acknowledge the Research Council of Azarbaijan Shahid Madani University for financial support.
Author information
Authors and Affiliations
Corresponding author
Electronic supplementary material
Below is the link to the electronic supplementary material.
Fig. S1
XRD patterns of graphene oxide (A) and hydrothermally reduced graphene oxide (B) (PDF 155 kb)
Rights and permissions
About this article
Cite this article
Mohammad-Rezaei, R., Razmi, H. & Jabbari, M. Graphene ceramic composite as a new kind of surface-renewable electrode: application to the electroanalysis of ascorbic acid. Microchim Acta 181, 1879–1885 (2014). https://doi.org/10.1007/s00604-014-1238-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s00604-014-1238-1