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Sensitive detection of hydrogen peroxide in foodstuff using an organic–inorganic hybrid multilayer-functionalized graphene biosensing platform

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Abstract

We report on a new electrochemical biosensing strategy for the sensitive detection of hydrogen peroxide (H2O2) in foodstuff samples. It is based on a gold electrode modified with layer of graphene patterned with a multilayer made from an organic–inorganic hybrid nanomaterial. Initially, a layer of thionine (Th) was assembled on the surface of the graphene nanosheets, and these were then cast on the surface of the electrode for the alternate assembly of gold nanoparticles and horseradish peroxidase. The large surface-to-volume ratio and high conductivity of the nanosheets provides a benign microenvironment for the construction of the biosensor. The use of such a multilayer not only shortens the electron transfer pathway of the active center of the enzyme due to the presence of gold nanoparticles, but also enhances the electrocatalytic efficiency of the biosensor toward the reduction of H2O2. The electrochemical characteristics of the biosensor were studied by cyclic voltammetry and chronoamperometry. The number of layers, the operating potential, and the pH of the supporting electrolyte were optimized. Linear response is obtained for the range from 0.5 μM to 1.8 mM of H2O2, the detection limit is 10 nM (at S/N = 3), and 95% of the steady-state current is reached within 2 s. The method was applied to sense H2O2 in spiked sterilized milk and correlated excellently with the permanganate titration method.

A new electrochemical biosensing strategy for sensitive detection of hydrogen peroxide in foodstuff was developed by using a gold electrode modified with a layer of graphene nanosheets patterned with a multilayer made from an organic–inorganic hybrid nanomaterial.

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References

  1. Chang Q, Deng K, Zhu L, Jiang G, Yu C, Tang H (2009) Determination of hydrogen peroxide with the aid of peroxidased-like Fe3O4 magnetic nanoparticles as the catalyst. Microchim Acta 165:299

    Article  CAS  Google Scholar 

  2. http://purehealthsystems.com/hydrogen-peroxide.html

  3. Young D, Mihaliak C, West S, Handelman K, Collins R, Phillips A, Robb C (2000) Determination of spinosad and its metabolites in food and environmental matrices. 3. Immunoassay methods. J Agric Food Chem 48:5146

    Article  CAS  Google Scholar 

  4. Xu S, Zhang X, Wan T, Zhang C (2011) A third-generation hydrogen peroxide biosensor based on horseradish peroxidase cross-linked to multi-wall carbon nanotubes. Microchim Acta 172:199

    Article  CAS  Google Scholar 

  5. Ping J, Ru S, Fan K, Wu J, Ying Y (2010) Copper oxide nanoparticles and ionic liquid modified carbon electrode for the non-enzymatic electrochemical sensing of hydrogen peroxide. Microchim Acta 171:117

    Article  CAS  Google Scholar 

  6. Che X, Yuan R, Chai Y, Ma L, Li W, Li J (2009) Hydrogen peroxide sensor based on horseradish peroxidase immobilized on an electrode modified with DNA-L-cysteine-gold-platinum nanoparticles in polypyrrole film. Microchim Acta 167:159

    Article  CAS  Google Scholar 

  7. Achatz D, Meier R, Fishcher L, Wolfbeis O (2011) Luminescent sensing of oxygen using a quenchable probe and upconverting nanoparticles. Angew Chem Int Ed 50:260

    Article  CAS  Google Scholar 

  8. Pumer M, Ambrosi A, Bonanni A, Chng E, Poh H (2010) Graphene for electrochemical sensing and biosensing. TrAC Anal Chem 29:954

    Article  Google Scholar 

  9. Willner I, Willner B, Tel-Vered R (2011) Electroanalytical applications of metallic nanoparticles and supramolecular nanostructurs. Electroanalysis 23:13

    Article  CAS  Google Scholar 

  10. Nikolelis D, Hianik T, Nikoleli G (2010) Stabilized lipid films in electrochemical biosensors. Electroanalysis 22:2747

    Article  CAS  Google Scholar 

  11. Lange U, Hirsch T, Mirsky V, Wolfbeis O (2011) Hydrogen sensor based on a graphene-palladium nanocomposite. Electrochim Acta. doi:10.1016/j.electacta.2010.10.078

    Google Scholar 

  12. Jia X, Campos-Delgado J, Terrones M, Meunier V, Dresselhaus M (2011) Graphene edges: a review of their fabrication and characterization. Nanoscale 3:86

    Article  CAS  Google Scholar 

  13. Mas-Balleste R, Gomez-Navarro C, Gomez-Herrero J, Zamora F (2011) 2D materials: to graphene and beyond. Nanoscale 3:20

    Article  CAS  Google Scholar 

  14. Brownson D, Banks C (2010) Graphene electrochemistry: an overview of potential applications. Analyst 135:2768

    Article  CAS  Google Scholar 

  15. Pumera M (2010) Graphene-based nanomaterials and their electrochemistry. Chem Soc Rev 39:4146

    Article  CAS  Google Scholar 

  16. Tosar J, Branas G, Laiz J (2010) Electrochemical DNA hybridization sensors applied to real and complex biological samples. Biosens Bioelectron 26:1205

    Article  CAS  Google Scholar 

  17. Suryanarayanan V, Wu C, Ho K (2010) Molecularly imprinted electrochemical sensors. Electroanalysis 22:1795

    Article  CAS  Google Scholar 

  18. Mantha S, Pedrosa V, Olsen E, Davis V, Simonian A (2010) Renewable nanocomposite layer-by-layer assembled catalytic interface for biosensing applications. Langmuir 26:19114

    Article  CAS  Google Scholar 

  19. Nguyen D, Kim D, Kim K (2011) Controlled synthesis and biomolecular probe application of gold nanoparticles. Micron 42:207

    Article  CAS  Google Scholar 

  20. Hayatt M (ed) (1989) Colloidal gold-principles, methods and applications. Academic, San Diego

    Google Scholar 

  21. Zhang Y, Tang Z, Fu X, Xu Y (2010) TiO2-graphene nanocomposites for gas-phase photocatalytic degradation of volatile aromatic pollutant: is TiO2-graphene truly different from other TiO2-carbon composite materials? ACS Nano 4:7303

    Article  CAS  Google Scholar 

  22. Turkevich J, Stevenson P, Hillier J (1951) A study of the nucleation and growth process in the synthesis of colloidal gold. Discuss Faraday Soc 11:55

    Article  Google Scholar 

  23. Frens G (1973) Controlled nucleation for the regulation of the particle size in monodisperse gold suspensions. Nat Phys Sci 241:20

    CAS  Google Scholar 

  24. Tang D, Tang J, Su B, Chen G (2011) Gold nanoparticles-decorated amine-terminated poly(amidoamine) dendrimer for sensitive electrochemical immunoassay of brevetoxins in food samples. Biosens Bioelectron 26:2090

    Article  CAS  Google Scholar 

  25. Tang D, Yuan R, Chai Y (2008) Ultrasensitive electrochemical immunosensor for clinical immunoassay using thionine-doped magnetic gold nanospheres as labels and horseradish peroxidase as enhancer. Anal Chem 80:1582

    Article  CAS  Google Scholar 

  26. Tang D, Yuan R, Chai Y (2006) Electrochemical immuno-bioanalysis for carcinoma antigen 125 based on thionine and gold nanoparticles modified carbon paste interface. Anal Chim Acta 564:158

    Article  CAS  Google Scholar 

  27. Tang D, Ren J (2008) In situ amplified electrochemical immunoassay for carcinoembryonic antigen using horseradish peroxidase-encapsulated nanogold hollow microspheres as labels. Anal Chem 80:8064

    Article  CAS  Google Scholar 

  28. Tang D, Yuan R, Chai Y (2006) Electron-transfer mediator microbiosensor fabrication based on immobilizing HRP-labeled Au colloids on gold electrode surface by 11-mercaptoundecanoic acid monolayer. Electroanalysis 18:259

    Article  CAS  Google Scholar 

  29. He Y, Zheng J, Li K, Sheng Q, Qiao N (2010) A hydrogen peroxide biosensor based on room temperature ionic liquid functionalized graphene modified carbon ceramic electrode. Chin J Chem 28:2507

    Article  CAS  Google Scholar 

  30. Zhang Y, Sun X, Zhu L, Shen H, Jia N (2011) Electrochemical sensing based on graphene/Prussian blue hybrid film modified electrode. Electrochim Acta 56:1239

    Article  CAS  Google Scholar 

  31. Xu J, Liu C, Wu Z (2011) Direct electrochemistry and enhanced electrocatalytic activity of hemoglobin entrapped in graphene and ZnO nanospheres composite film. Microchim Acta. doi:10.1007/s00604-010-0515-x

    Google Scholar 

  32. Zhou Y, Liu S, Jiang H, Yang H, Chen H (2010) Direct electrochemistry and bioelectrocatalysis of microperoxidase-11 immobilized on chitosan-graphene nanocomposites. Electroanalysis 22:1323

    Article  CAS  Google Scholar 

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Acknowledgement

The support by the National Natural Science Foundation of China (21075019, 20735002), the Research Fund for the Doctoral Program of Higher Education of China (20103514120003), the “973” National Basic Research Program of China (2010CB732403), and Program for Returned High-Level Overseas Chinese Scholars of Fujian Province (XRC-0929) is gratefully acknowledged.

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Correspondence to Dianping Tang.

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Cui, Y., Zhang, B., Liu, B. et al. Sensitive detection of hydrogen peroxide in foodstuff using an organic–inorganic hybrid multilayer-functionalized graphene biosensing platform. Microchim Acta 174, 137–144 (2011). https://doi.org/10.1007/s00604-011-0608-1

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