Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide
High potential purified Trametes trogii laccase has been studied as a biocatalyst for oxygen cathodes composed of layer-by-layer self-assembled thin films by sequential immersion of mercaptopropane sulfonate-modified Au electrode surfaces in solutions containing laccase and osmium-complex bound to p...
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todo:paper_00027863_v132_n32_p11132_Scodeller2023-10-03T13:54:14Z Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide Scodeller, P. Carballo, R. Szamocki, R. Levin, L. Forchiassin, F. Calvo, E.J. Au electrodes Biofuel cell Current dependence High potential Inhibitory effect Kinetic evidence Laccases Layer-by-layers Mass transport Negative charge Oxygen cathodes Oxygen partial pressure Oxygen Reduction Peak shapes Polarization curves Poly(allylamine) Polyanions Polycations Rotating disk electrodes Scanning electrochemical microscopy Self assembled thin film Self-assembled Biofuels Biological fuel cells Cathodes Cyclic voltammetry Electrocatalysis Electrochemical electrodes Electrolytic reduction Enzymes Hydrogen peroxide Organic polymers Osmium Oxidation Oxide minerals Oxygen Quartz Rotating disks Scanning electron microscopy Scanning probe microscopy Thin films Gold allylamine derivative biofuel gold hydrogen peroxide laccase osmium oxygen polymer self assembled monolayer thiol derivative article biocatalysis biocatalyst biofuel cell electrode energy resource enzyme activity hysteresis kinetics oxidation reduction reaction oxygen tension Trametes Biocatalysis Bioelectric Energy Sources Diffusion Electrodes Hydrogen Peroxide Kinetics Laccase Microscopy, Electron, Scanning Osmium Oxidation-Reduction Oxygen Polymers Pressure Rotation Trametes High potential purified Trametes trogii laccase has been studied as a biocatalyst for oxygen cathodes composed of layer-by-layer self-assembled thin films by sequential immersion of mercaptopropane sulfonate-modified Au electrode surfaces in solutions containing laccase and osmium-complex bound to poly(allylamine), (PAH-Os). The polycation backbone carries the Os redox relay, and the polyanion is the enzyme adsorbed from a solution of a suitable pH so that the protein carries a net negative charge. Enzyme thin films were characterized by quartz crystal microbalance, ellipsometry, cyclic voltammetry, and oxygen reduction electrocatalysis under variable oxygen partial pressures with a rotating disk electrode. New kinetic evidence relevant to biofuel cells is presented on the detection of traces of H2O2, intermediate in the O2 reduction, with scanning electrochemical microscopy (SECM). Furthermore the inhibitory effect of peroxide on the biocatalytic current resulted in abnormal current dependence on the O 2 partial pressure and peak shape with hysteresis in the polarization curves under stagnant conditions, which is offset upon stirring with the RDE. The new kinetic evidence reported in the present work is very relevant for the operation of biofuel cells under stagnant conditions of O2 mass transport. © 2010 American Chemical Society. Fil:Scodeller, P. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Levin, L. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Forchiassin, F. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Calvo, E.J. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_00027863_v132_n32_p11132_Scodeller |
| institution |
Universidad de Buenos Aires |
| institution_str |
I-28 |
| repository_str |
R-134 |
| collection |
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| topic |
Au electrodes Biofuel cell Current dependence High potential Inhibitory effect Kinetic evidence Laccases Layer-by-layers Mass transport Negative charge Oxygen cathodes Oxygen partial pressure Oxygen Reduction Peak shapes Polarization curves Poly(allylamine) Polyanions Polycations Rotating disk electrodes Scanning electrochemical microscopy Self assembled thin film Self-assembled Biofuels Biological fuel cells Cathodes Cyclic voltammetry Electrocatalysis Electrochemical electrodes Electrolytic reduction Enzymes Hydrogen peroxide Organic polymers Osmium Oxidation Oxide minerals Oxygen Quartz Rotating disks Scanning electron microscopy Scanning probe microscopy Thin films Gold allylamine derivative biofuel gold hydrogen peroxide laccase osmium oxygen polymer self assembled monolayer thiol derivative article biocatalysis biocatalyst biofuel cell electrode energy resource enzyme activity hysteresis kinetics oxidation reduction reaction oxygen tension Trametes Biocatalysis Bioelectric Energy Sources Diffusion Electrodes Hydrogen Peroxide Kinetics Laccase Microscopy, Electron, Scanning Osmium Oxidation-Reduction Oxygen Polymers Pressure Rotation Trametes |
| spellingShingle |
Au electrodes Biofuel cell Current dependence High potential Inhibitory effect Kinetic evidence Laccases Layer-by-layers Mass transport Negative charge Oxygen cathodes Oxygen partial pressure Oxygen Reduction Peak shapes Polarization curves Poly(allylamine) Polyanions Polycations Rotating disk electrodes Scanning electrochemical microscopy Self assembled thin film Self-assembled Biofuels Biological fuel cells Cathodes Cyclic voltammetry Electrocatalysis Electrochemical electrodes Electrolytic reduction Enzymes Hydrogen peroxide Organic polymers Osmium Oxidation Oxide minerals Oxygen Quartz Rotating disks Scanning electron microscopy Scanning probe microscopy Thin films Gold allylamine derivative biofuel gold hydrogen peroxide laccase osmium oxygen polymer self assembled monolayer thiol derivative article biocatalysis biocatalyst biofuel cell electrode energy resource enzyme activity hysteresis kinetics oxidation reduction reaction oxygen tension Trametes Biocatalysis Bioelectric Energy Sources Diffusion Electrodes Hydrogen Peroxide Kinetics Laccase Microscopy, Electron, Scanning Osmium Oxidation-Reduction Oxygen Polymers Pressure Rotation Trametes Scodeller, P. Carballo, R. Szamocki, R. Levin, L. Forchiassin, F. Calvo, E.J. Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| topic_facet |
Au electrodes Biofuel cell Current dependence High potential Inhibitory effect Kinetic evidence Laccases Layer-by-layers Mass transport Negative charge Oxygen cathodes Oxygen partial pressure Oxygen Reduction Peak shapes Polarization curves Poly(allylamine) Polyanions Polycations Rotating disk electrodes Scanning electrochemical microscopy Self assembled thin film Self-assembled Biofuels Biological fuel cells Cathodes Cyclic voltammetry Electrocatalysis Electrochemical electrodes Electrolytic reduction Enzymes Hydrogen peroxide Organic polymers Osmium Oxidation Oxide minerals Oxygen Quartz Rotating disks Scanning electron microscopy Scanning probe microscopy Thin films Gold allylamine derivative biofuel gold hydrogen peroxide laccase osmium oxygen polymer self assembled monolayer thiol derivative article biocatalysis biocatalyst biofuel cell electrode energy resource enzyme activity hysteresis kinetics oxidation reduction reaction oxygen tension Trametes Biocatalysis Bioelectric Energy Sources Diffusion Electrodes Hydrogen Peroxide Kinetics Laccase Microscopy, Electron, Scanning Osmium Oxidation-Reduction Oxygen Polymers Pressure Rotation Trametes |
| description |
High potential purified Trametes trogii laccase has been studied as a biocatalyst for oxygen cathodes composed of layer-by-layer self-assembled thin films by sequential immersion of mercaptopropane sulfonate-modified Au electrode surfaces in solutions containing laccase and osmium-complex bound to poly(allylamine), (PAH-Os). The polycation backbone carries the Os redox relay, and the polyanion is the enzyme adsorbed from a solution of a suitable pH so that the protein carries a net negative charge. Enzyme thin films were characterized by quartz crystal microbalance, ellipsometry, cyclic voltammetry, and oxygen reduction electrocatalysis under variable oxygen partial pressures with a rotating disk electrode. New kinetic evidence relevant to biofuel cells is presented on the detection of traces of H2O2, intermediate in the O2 reduction, with scanning electrochemical microscopy (SECM). Furthermore the inhibitory effect of peroxide on the biocatalytic current resulted in abnormal current dependence on the O 2 partial pressure and peak shape with hysteresis in the polarization curves under stagnant conditions, which is offset upon stirring with the RDE. The new kinetic evidence reported in the present work is very relevant for the operation of biofuel cells under stagnant conditions of O2 mass transport. © 2010 American Chemical Society. |
| format |
JOUR |
| author |
Scodeller, P. Carballo, R. Szamocki, R. Levin, L. Forchiassin, F. Calvo, E.J. |
| author_facet |
Scodeller, P. Carballo, R. Szamocki, R. Levin, L. Forchiassin, F. Calvo, E.J. |
| author_sort |
Scodeller, P. |
| title |
Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| title_short |
Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| title_full |
Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| title_fullStr |
Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| title_full_unstemmed |
Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide |
| title_sort |
layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: the role of hydrogen peroxide |
| url |
http://hdl.handle.net/20.500.12110/paper_00027863_v132_n32_p11132_Scodeller |
| work_keys_str_mv |
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| _version_ |
1782024102046859264 |