Simulation of multistep enzyme-catalyzed methanol oxidation in biofuel Cells

Piyush Kar, Hao Wen, Hanzi Li, Shelley D. Minteer, Scott Calabrese Barton

    Research output: Contribution to journalArticle

    • 28 Citations

    Abstract

    We report a simulation of multi-step enzyme catalysis and cofactor-mediated electron transfer in a bio-anode of a methanol biofuel cell. Three nicotinamide adenine dinucleotide (NAD+) dependent dehydrogenase enzymes, namely alcohol dehydrogenase (ADH), aldehyde dehydrogenase (AlDH), and formate dehydrogenase (FDH) combine to achieve complete oxidation of methanol to carbon dioxide. Oxidation of methanol by the enzyme cascade produces the reduced co-factor, NADH, which is oxidized to regenerate NAD+ at an electrode comprised of a poly(methylene green) catalyst electrodeposited on carbon paper. Kinetic parameters for the enzymatic oxidation reactions were experimentally determined between pH 6.5 and 9 and were employed in the simulation to evaluate the effect of pH. Model results compare closely to previously reported experimental data over a broad pH range. Model-based analysis indicates that cell performance is controlled by NAD+ transport and NADH oxidation kinetics for electrode specific areas lower than 3 m2+ cm -3 and shifted to enzyme kinetic control at higher specific area. An optimal electrode design is predicted to achieve current density exceeding 10 mA cm-2.

    Original languageEnglish (US)
    JournalJournal of the Electrochemical Society
    Volume158
    Issue number5
    DOIs
    StatePublished - 2011

    Profile

    enzymes
    oxidation
    Oxidation
    Avian Leukosis
    dehydrogenases
    methyl alcohol
    Methanol
    Enzymes
    electrodes
    kinetics
    cells
    simulation
    Electrodes
    Autoradiography
    Biological fuel cells
    Carubicin
    Anthralin
    nicotinamide
    adenines
    formates

    ASJC Scopus subject areas

    • Electrochemistry
    • Electronic, Optical and Magnetic Materials
    • Materials Chemistry
    • Surfaces, Coatings and Films
    • Renewable Energy, Sustainability and the Environment
    • Condensed Matter Physics

    Cite this

    Simulation of multistep enzyme-catalyzed methanol oxidation in biofuel Cells. / Kar, Piyush; Wen, Hao; Li, Hanzi; Minteer, Shelley D.; Calabrese Barton, Scott.

    In: Journal of the Electrochemical Society, Vol. 158, No. 5, 2011.

    Research output: Contribution to journalArticle

    Kar, Piyush; Wen, Hao; Li, Hanzi; Minteer, Shelley D.; Calabrese Barton, Scott / Simulation of multistep enzyme-catalyzed methanol oxidation in biofuel Cells.

    In: Journal of the Electrochemical Society, Vol. 158, No. 5, 2011.

    Research output: Contribution to journalArticle

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    abstract = "We report a simulation of multi-step enzyme catalysis and cofactor-mediated electron transfer in a bio-anode of a methanol biofuel cell. Three nicotinamide adenine dinucleotide (NAD+) dependent dehydrogenase enzymes, namely alcohol dehydrogenase (ADH), aldehyde dehydrogenase (AlDH), and formate dehydrogenase (FDH) combine to achieve complete oxidation of methanol to carbon dioxide. Oxidation of methanol by the enzyme cascade produces the reduced co-factor, NADH, which is oxidized to regenerate NAD+ at an electrode comprised of a poly(methylene green) catalyst electrodeposited on carbon paper. Kinetic parameters for the enzymatic oxidation reactions were experimentally determined between pH 6.5 and 9 and were employed in the simulation to evaluate the effect of pH. Model results compare closely to previously reported experimental data over a broad pH range. Model-based analysis indicates that cell performance is controlled by NAD+ transport and NADH oxidation kinetics for electrode specific areas lower than 3 m2+ cm -3 and shifted to enzyme kinetic control at higher specific area. An optimal electrode design is predicted to achieve current density exceeding 10 mA cm-2.",
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