Development of novel bioelectrocatalytic systems through controlled combination of multiwalled carbon nanotubes, redox mediators and enzymes

Paweł J. Kulesza ,  Barbara Kowalewska 

University of Warsaw, Faculty of Chemistry, Pasteura1, Warsaw 02-093, Poland

Recently, multi-walled carbon nanotubes (MCNT) have gained considerable attention, because of their remarkable electronic and mechanical properties, which have made them extremely attractive for a wide range of sensing applications from structural materials to nanoelectronic components. The ability of MCNT modified electrodes to promote electron transfer reactions has been documented in connection with important biomolecules [1]. Our goal is to explore new applications of MCNT as a electrode material in facilitating the electron transfer between biomolecules and electrode in bioelectrocatalytic systems of potential utility for biofuel cells.

This lecture will give an overview and discuss anode and cathode reactions based on multi-component films for oxygen and hydrogen peroxide reduction and fuel oxidation. Cathode reactions will cover those based on Co-porphyrin centers that are expected to induce reduction of oxygen at the initial stage, and the enzyme (horseradish or cabbage peroxidase) that should act as highly reactive catalyst capable of further reducing hydrogen peroxide intermediate [2]. The multi component bioelectrocatalytic film has also exhibited relatively higher activity towards reduction of hydrogen peroxide. Anode reactions will cover those based on mediated electron transfer. The presence of mediator is expected to facilitate an effective flow of electrons from the redox centers of glucose oxidase to the glassy carbon electrode.

We have also considered utilizing new enzymes to design, characterize and evaluate different types and distinct configurations of enzyme-based multi-component and well organized bioelectrocatalytic systems capable of effective oxidation of ethanol in neutral media. At all stages of investigations, comparison have been made to the behavior (under analogous conditions) of glucose with glucose oxidase as model enzyme [3]. A special attention have been paid to development of mediation and enzyme immobilization methodology for continuous and efficient electron transfer from the enzyme to the electrode surface.

On the whole, a stable multifunctional composite bio-electrocatalytic films for fuel oxidation and oxygen reduction under neutral conditions are produced. Finally, the formation, morphology, structural transformations and electrochemical properties of the MCNT-containing three-dimensional network films have been examined using cyclic voltammetry, potential step techniques, rotating disc voltammetry, FTIR spectroscopy and tranmission electron microscopy. The ability to create bioelectrocatalytic nanocomposites provides an opportunity to construct functional bioanodes and biocathodes. Follow on research will use the approach to design a biofuel cell system that utilizes an nanostructured enzyme-based anode and cathode working in tandem.



[1] J.J. Gooding, R.Wibowo, J. Liu, W. Yang, D. Losic, S.Orbons, F.J. Mearns, J.G. Shapter, D.B. Ilibbert, J. Am. Chem. Soc., 125 (2003) 9006.

[2] B. Kowalewska, M. Skunik, K. Karnicka, K. Miecznikowski, M. Chojak, G. Ginalska, A. Belcarz, P. J. Kulesza, Electrochim. Acta, 53 (2008) 2408.

[3] B. Kowalewska, P.J. Kulesza, Electroanalysis, 21 (2009) 351.

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Presentation: Keynote lecture at SMCBS'2009 International Workshop, by Paweł J. Kulesza
See On-line Journal of SMCBS'2009 International Workshop

Submitted: 2009-09-07 19:29
Revised:   2009-09-07 19:31
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