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One-pot sonocatalyzed synthesis of sol–gel graphite electrodes containing gold nanoparticles for application in amperometric sensing

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Abstract

We propose here a one-pot synthetic approach to prepare sol–gel graphite electrodes containing gold nanoparticles (AuNPs). At variance with the traditional synthesis, in which AuNPs are prepared in advance with respect to the silica matrix, they were here obtained directly inside the sol–gel, during its formation. Two reduction methods, namely chemical and thermal reduction, were used to achieve AuNPs starting from a suitable gold precursor, either consisting of NaAuCl4 or HAuCl4. Different experimental parameters were tested in order to direct the synthesis of the material to the characteristics sought, namely Si/Au molar ratio, graphite (g): silane precursor (mL) ratio, chemical nature of the gold precursor and of the reductant, duration and temperature of thermal treatment. Sol–gel was prepared by means of sonocatalysis, in order to reduce the amount of solvent and time necessary for the hydrolysis step. Composition of the material, as well as shape, size and distribution of AuNPs inside the silica matrix was evaluated by spectroscopic and microscopic techniques. Furthermore, electrochemical tests allowed us to ascertain the good conductivity of the composite material and the electrocatalytic activity of AuNPs with respect to glucose and ascorbic acid oxidation. These tests demonstrated that the electrodes obtained by thermal reduction show the best performance in terms of sensitivity for the detection of these analytes, suggesting the possible application of this composite in the field of amperometric sensing.

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References

  1. Tsionsky M, Gun M, Glezer M, Lev O (1994) Sol-gel-derived ceramic-carbon composite electrodes: introduction and scope of applications. Anal Chem 66:1747–1753

    Article  Google Scholar 

  2. Lev O, Tsionsky M, Rabinovich L, Glezer V, Sampath S, Pankratov I, Gun J (1995) Organically modified sol-gel sensors. Anal Chem 67:22A–30A

    Article  Google Scholar 

  3. Collinson MM, Howells AR (2000) Sol–gels and electrochemistry: research at the intersection. Anal Chem 72:702A–709A

    Google Scholar 

  4. Rabinovich L, Lev O (2001) Sol–gel derived composite ceramic carbon electrodes. Electroanal Int J Devoted Fundam Pract Asp Electroanal 13:265–275

    Google Scholar 

  5. Walcarius A, Mandler D, Cox JA, Collinson M, Lev O (2005) Exiting new directions in the intersection of functionalized sol–gel materials with electrochemistry. J Mater Chem 15:3663–3689

    Article  Google Scholar 

  6. Walcarius A (2001) Electroanalysis with pure, chemically modified, and sol–gel-derived silica-based materials. Electroanal Int J Devoted Fundam Pract Asp Electroanal 13:701–718

    Google Scholar 

  7. Walcarius A (2018) Silica-based electrochemical sensors and biosensors: recent trends. Curr Opin Electrochem 10:88–97

    Article  Google Scholar 

  8. Seeber R, Terzi F, Zanardi C (2014) Functional materials in amperometric sensing: polymeric, inorganic, and nanocomposite materials for modified electrodes. Springer, Heidelberg

    Book  Google Scholar 

  9. Juan-Díaz MJ, Martínez-Ibánez M, Hernández-Escolano M, Cabedo L, Izquierdo R, Suay J, Gurruchaga J, Goni I (2014) Study of the degradation of hybrid sol–gel coatings in aqueous medium. Prog Org Coat 77:1799–1806

    Article  Google Scholar 

  10. Brinker CJ, Scherer GW (1990) Sol gel science: the physic and chemistry of sol–gel processing. Academic Press Inc., New York

    Google Scholar 

  11. Cordero-Rando MM, Hidalgo-Hidalgo de Cisneros JL, Blanco E, Narajo-Rodriguez I (2002) The sonogel-carbon electrode as a sol–gel graphite-based electrode. Anal Chem 74:2423–2427

    Article  Google Scholar 

  12. Ballarin B, Zanardi C, Schenetti L, Seeber R, Hidalgo-Hidalgo de Cisneros JL (2003) Synthesis and electrochemical characterisation of novel sonogel-carbon-polythiophene microstructured electrodes. Synth Metals 139:29–33

    Article  Google Scholar 

  13. Abdelrahim MYM, Benjamin SR, Cubillana-Aguilera LM et al (2013) Study of electrocatalytic activity of cerium oxide and gold-studded cerium oxide nanoparticles using a sono-gel-carbon material as supporting electrode: electroanalytical study in apple juice for babies. Sensors 13:4979–5007

    Article  Google Scholar 

  14. Crespo-Rosa JR, Zanardi C, ElKaouitit M, Terzi F, Seeber R, Naranjo-Rodriguez I (2014) Electroanalytical applications of a graphite-Au nanoparticles composite included in a sonogel matrix. Electrochim Acta 122:310–315

    Article  Google Scholar 

  15. Daniel M-C, Astruc D (2014) Gold nanoparticles: assembly, supramolecular chemistry, quantum-size-related properties, and applications toward biology, catalysis, and nanotechnology. Chem Rev 104:293–346

    Article  Google Scholar 

  16. Wang J, Pamidi PVA (1997) Sol–gel-derived gold composite electrodes. Anal Chem 69:4490–4494

    Article  Google Scholar 

  17. Jena BR, Raj CR (2006) Enzyme-free amperometric sensing of glucose by using gold nanoparticles. Chem Eur J 12:2702–2708

    Article  Google Scholar 

  18. Maduraiveeran G, Ramaraj R (1951) Gold nanoparticles embedded in silica sol-gel matrix as amperometric sensor for hydrogen peroxide. J Electroanal Chem 608:52–58

    Article  Google Scholar 

  19. Turkevich J, Stevenson PC, Hillier J (1951) A study of the nucleation and growth processes in the synthesis of colloidal gold. Discuss Faraday Soc 11:55–75

    Article  Google Scholar 

  20. McFarland AD, Haynes CL, Mirkin CA, Van Duyne RP, Godwin HA (2004) Color my nanoworld. J Chem Educ 81:544A–544B

    Article  Google Scholar 

  21. Lusvardi G, Malavasi G, Menabue L, Aina V, Bertinetti L, Cerrato G, Morterra C (2010) Bioactive glasses containing Au nanoparticles. Effect of calcination temperature on structure, morphology, and surface properties. Langmuir 26:10303–10314

    Article  Google Scholar 

  22. Larew LA, Johnson DC (1989) Concentration dependence of the mechanism of glucose oxidation at gold electrodes in alkaline media. J Electroanal Chem 262:167–182

    Article  Google Scholar 

  23. Burke LD, Ryan TG (1992) The role of incipient hydrous oxides in the oxidation of glucose and some of its derivatives in aqueous media. Electrochim Acta 37:1363–1370

    Article  Google Scholar 

  24. Bello A, Giannetto M, Mori G, Seeber R, Terzi F, Zanardi C (2007) Optimization of the DPV potential waveform for determination of ascorbic acid on PEDOT-modified electrodes. Sens Act B 121:430–435

    Article  Google Scholar 

  25. Zhao J, Griederich B (2015) Synthesis of gold nanoparticles via chemical reduction methods. In: 7th Nanocon, Brno, Czech Republic, EU

  26. Rasband W, ImageJ Version 1.32J, National Institute of Mental Health, Bethesda, Maryland, USA

  27. Gwyddion Version 2.53. http://gwyddion.net/. Accessed 2 Apr 2019

  28. Angerstein-Kozlowska H, Conway BE, Hamelin A, Stoicoviciu L (1987) Filamentary steps of electrochemical oxidation of single crystal planes of Au. Part II: a chemical and structural basis of oxidation of the (111) plane. J Electroanal Chem 228:429–453

    Article  Google Scholar 

  29. PCPFWIN 2.3. JCPDS International center for diffraction data, 637 Swarthmore 2002

  30. Toghill KE, Compton RG (2010) Electrochemical non-enzymatic glucose sensors: a perspective and an evaluation. Int J Electrochem Sci 5:1246–1301

    Google Scholar 

  31. Rueda M, Aldaz A, Sanchez-Burws F (1978) Oxidation of L-ascorbic acid on a gold electrode. Electrochim Acta 23:419–424

    Article  Google Scholar 

  32. Hu IF, Kuwana T (1986) Oxidative mechanism of ascorbic acid at glassy carbon electrodes. Anal Chem 58:3235–3239

    Article  Google Scholar 

  33. Manzanares MI, Solfs V, de Rossi RH (1986) Effect of cyclodextrins on the electrochemical behaviour of ascorbic acid on gold electrodes. J Electroanal Chem 407:141–147

    Article  Google Scholar 

  34. Zanardi C, Terzi F, Seeber R (2010) Composite electrode coatings in amperometric sensors. Effects of differently encapsulated gold nanoparticles in poly(3,4-ethylendioxythiophene) system. Sens Actuators B 148:277–282

    Article  Google Scholar 

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Acknowledgements

This research was financed with funds from the University of Modena e Reggio Emilia, (Project FAR 2015, “Sviluppo Di Materiali A Base Silicatica Per Applicazioni Sensoristiche” Decreto rettorale n. 267/2016 Prot. n. 81676 del 28/06/2016). Authors also thank the “Centro Interdipartimentale Grandi Strumenti” (CIGS) of the University of Modena e Reggio Emilia for instrument availability and assistance.

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  1. Department of Chemical and Geological Sciences, University of Modena e Reggio Emilia, Via G. Campi 103, 41125, Modena, Italy

    Maria Laura Ligabue, Fabio Terzi, Chiara Zanardi & Gigliola Lusvardi

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  1. Maria Laura Ligabue
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  2. Fabio Terzi
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  3. Chiara Zanardi
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  4. Gigliola Lusvardi
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Correspondence to Chiara Zanardi or Gigliola Lusvardi.

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Ligabue, M.L., Terzi, F., Zanardi, C. et al. One-pot sonocatalyzed synthesis of sol–gel graphite electrodes containing gold nanoparticles for application in amperometric sensing. J Mater Sci 54, 9553–9564 (2019). https://doi.org/10.1007/s10853-019-03580-y

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