Performance of non-compartmentalized enzymatic biofuel cell based on buckypaper cathode and ferrocene-containing redox polymer anode

Abstract Novel single compartment Glucose/O2 biofuel cells (BFCs) were developed using immobilized enzymes and the mediated electron transfer (MET) approach. The bioanode was prepared through a ferrocene-containing redox polymer crosslinked in the presence of a biocatalyst on a glassy carbon support. Here, the redox polymer can physically entrap the enzyme and prevent it from leaching. Additionally it provides a biocompatible microenvironment and thus could extend the life time of enzyme. On the other side, the mediated biocathode was prepared based on bilirubin oxidase and 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonate) diammonium salt (ABTS2−) system which has been physically entrapped in Nafion matrix and then adsorbed directly on a highly porous, conductive and functionalized buckypaper (fBP). Both electrodes were characterized physically and electrochemically. Employing these electrodes, the resulting BFC generates an open circuit voltage (Voc) of approximately 0.550 V and a peak power density of 26 μW cm−2 at 0.2 V at 37 °C in quiescent O2-saturated physiological buffer containing 5 mM glucose. The cell sustains a load up to 225 μA cm−2. Moreover, a high short circuit current (Isc) of 300 μA cm−2 is approached. This BFC can operate in mild conditions without using any toxic materials which makes it attractive for implantable devices.

[1]  Katz,et al.  Integration of Layered Redox Proteins and Conductive Supports for Bioelectronic Applications. , 2000, Angewandte Chemie.

[2]  Adam Heller,et al.  A laccase-wiring redox hydrogel for efficient catalysis of O2 electroreduction. , 2006, The journal of physical chemistry. B.

[3]  A. Turner,et al.  Ferrocene-mediated enzyme electrode for amperometric determination of glucose. , 1984, Analytical chemistry.

[4]  F. Gao,et al.  Engineering hybrid nanotube wires for high-power biofuel cells. , 2010, Nature communications.

[5]  Shelley D. Minteer,et al.  Development of alcohol/O2 biofuel cells using salt-extracted tetrabutylammonium bromide/Nafion membranes to immobilize dehydrogenase enzymes , 2005 .

[6]  Adam Heller,et al.  A Miniature Membrane-less Biofuel Cell Operating under Physiological Conditions at 0.5 V , 2003 .

[7]  J. Rühe,et al.  Photochemical generation of ferrocene-based redox-polymer networks. , 2009, Macromolecular rapid communications.

[8]  C. Danilowicz,et al.  Electrical Communication between Electrodes and Enzymes Mediated by Redox Hydrogels. , 1996, Analytical chemistry.

[9]  Matthew B. Johnson,et al.  Effect of Mediator Spacing on Electrochemical and Enzymatic Response of Ferrocene Redox Polymers , 2010 .

[10]  L. Gorton,et al.  Wiring of pyranose dehydrogenase with osmium polymers of different redox potentials. , 2010, Bioelectrochemistry.

[11]  Adam Heller,et al.  Integrated medical feedback systems for drug delivery , 2005 .

[12]  Adam Heller,et al.  Redox polymer films containing enzymes. 2. Glucose oxidase containing enzyme electrodes , 1991 .

[13]  Itamar Willner,et al.  A non-compartmentalized glucose ∣ O2 biofuel cell by bioengineered electrode surfaces , 1999 .

[14]  Philippe Cinquin,et al.  Mediatorless high-power glucose biofuel cells based on compressed carbon nanotube-enzyme electrodes , 2011, Nature communications.

[15]  G. Tayhas R. Palmore,et al.  Electro-enzymatic reduction of dioxygen to water in the cathode compartment of a biofuel cell , 1999 .

[16]  N. Mano,et al.  Characteristics of a miniature compartment-less glucose-O2 biofuel cell and its operation in a living plant. , 2003, Journal of the American Chemical Society.

[17]  M. M. Abd-Elzaher,et al.  On the medicinal chemistry of ferrocene , 2007 .

[18]  J. Rühe,et al.  Printed protein microarrays on unmodified plastic substrates. , 2010, Analytica chimica acta.

[19]  Robert K. Murray,et al.  Harper's Illustrated Biochemistry , 2003 .

[20]  H. Hill,et al.  Amperometric enzyme electrodes , 1986 .

[21]  José L. Fernández,et al.  Oxygen is electroreduced to water on a "wired" enzyme electrode at a lesser overpotential than on platinum. , 2003, Journal of the American Chemical Society.

[22]  A. Heller Miniature biofuel cells , 2004 .

[23]  Tobias A. F. König,et al.  Enzyme containing redox polymer networks for biosensors or biofuel cells: a photochemical approach. , 2010, Langmuir : the ACS journal of surfaces and colloids.

[24]  Shelley D Minteer,et al.  Extended lifetime biofuel cells. , 2008, Chemical Society reviews.

[25]  Adam Heller,et al.  A four-electron O(2)-electroreduction biocatalyst superior to platinum and a biofuel cell operating at 0.88 V. , 2004, Journal of the American Chemical Society.

[26]  G. Urban,et al.  Functionalized-carbon nanotube supported electrocatalysts and buckypaper-based biocathodes for glucose fuel cell applications , 2011 .

[27]  J. Gallaway,et al.  Effect of redox polymer synthesis on the performance of a mediated laccase oxygen cathode , 2009 .

[28]  V. Flexer,et al.  Oxygen cathode based on a layer-by-layer self-assembled laccase and osmium redox mediator , 2009 .

[29]  Eugenii Katz,et al.  Improving enzyme–electrode contacts by redox modification of cofactors , 1995, Nature.

[30]  Adam Heller,et al.  Electrical Wiring of Glucose Oxidase by Reconstitution of FAD-Modified Monolayers Assembled onto Au-Electrodes , 1996 .

[31]  F. Armstrong,et al.  Enzymes as working or inspirational electrocatalysts for fuel cells and electrolysis. , 2008, Chemical reviews.

[32]  G. Urban,et al.  Fabrication and characterization of buckypaper-based nanostructured electrodes as a novel material for biofuel cell applications. , 2011, Physical chemistry chemical physics : PCCP.

[33]  Adam Heller,et al.  Electron-conducting redox hydrogels: Design, characteristics and synthesis. , 2006, Current opinion in chemical biology.

[34]  P. Atanassov,et al.  Oxygen-reducing enzyme cathodes produced from SLAC, a small laccase from Streptomyces coelicolor. , 2008, Biosensors & bioelectronics.

[35]  G. Urban,et al.  A highly efficient buckypaper-based electrode material for mediatorless laccase-catalyzed dioxygen reduction. , 2011, Biosensors & bioelectronics.

[36]  N. Mano,et al.  Designing highly efficient enzyme-based carbonaceous foams electrodes for biofuel cells , 2010 .

[37]  Itamar Willner,et al.  Integrated oligoaniline-cross-linked composites of Au nanoparticles/glucose oxidase electrodes: a generic paradigm for electrically contacted enzyme systems. , 2009, Chemistry.

[38]  J. Rogalski,et al.  Enzymatic electrodes nanostructured with functionalized carbon nanotubes for biofuel cell applications , 2010, Analytical and bioanalytical chemistry.

[39]  A. Cass,et al.  Ferricinium ion as an electron acceptor for oxido-reductases , 1985 .

[40]  J. Rühe,et al.  Swelling Behavior of Thin, Surface-Attached Polymer Networks , 2004 .

[41]  Itamar Willner,et al.  Nano-engineered flavin-dependent glucose dehydrogenase/gold nanoparticle-modified electrodes for glucose sensing and biofuel cell applications. , 2011, ACS nano.

[42]  Adam Heller,et al.  Electrochemical glucose sensors and their applications in diabetes management. , 2008, Chemical reviews.

[43]  David M J S Bowman,et al.  Flammable biomes dominated by eucalypts originated at the Cretaceous-Palaeogene boundary. , 2011, Nature communications.

[44]  J. Rühe,et al.  Synthesis of Functionalized Polymer Monolayers from Active Ester Brushes , 2007 .

[45]  A. English,et al.  Characterization of a Ferrocene-Containing Polyacrylamide-Based Redox Gel for Biosensor Use , 1995 .

[46]  D. Glatzhofer,et al.  Effects of electrolyte and pH on the behavior of cross-linked films of ferrocene-modified poly(ethylenimine). , 2007, Langmuir : the ACS journal of surfaces and colloids.

[47]  N. Lewis,et al.  Powering the planet: Chemical challenges in solar energy utilization , 2006, Proceedings of the National Academy of Sciences.

[48]  Christopher F Blanford,et al.  Efficient electrocatalytic oxygen reduction by the 'blue' copper oxidase, laccase, directly attached to chemically modified carbons. , 2008, Faraday discussions.

[49]  Plamen Atanassov,et al.  Glucose oxidase anode for biofuel cell based on direct electron transfer , 2006 .

[50]  Takeo Yamaguchi,et al.  High-Surface-Area Three-Dimensional Biofuel Cell Electrode Using Redox-Polymer-Grafted Carbon , 2006 .