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Abstract:

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.

Registro:

Documento: Artículo
Título:Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide
Autor:Scodeller, P.; Carballo, R.; Szamocki, R.; Levin, L.; Forchiassin, F.; Calvo, E.J.
Filiación:INQUIMAE-DQIAyQF, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, 1428 Buenos Aires, Argentina
Micología Experimental, Departamento de Biodiversidad y Biología Experimental, Universidad de Buenos Aires, 1428 Buenos Aires, Argentina
Saarland University, 66123 Saarbrücken, Germany
Palabras clave: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
Año:2010
Volumen:132
Número:32
Página de inicio:11132
Página de fin:11140
DOI: http://dx.doi.org/10.1021/ja1020487
Título revista:Journal of the American Chemical Society
Título revista abreviado:J. Am. Chem. Soc.
ISSN:00027863
CODEN:JACSA
CAS:gold, 7440-57-5; hydrogen peroxide, 7722-84-1; laccase, 80498-15-3; osmium, 7440-04-2; oxygen, 7782-44-7; thiol derivative, 13940-21-1; Hydrogen Peroxide, 7722-84-1; Laccase, 1.10.3.2; Osmium, 7440-04-2; Oxygen, 7782-44-7; Polymers
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00027863_v132_n32_p11132_Scodeller

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Citas:

---------- APA ----------
Scodeller, P., Carballo, R., Szamocki, R., Levin, L., Forchiassin, F. & Calvo, E.J. (2010) . Layer-by-layer self-assembled osmium polymer-mediated laccase oxygen cathodes for biofuel cells: The role of hydrogen peroxide. Journal of the American Chemical Society, 132(32), 11132-11140.
http://dx.doi.org/10.1021/ja1020487
---------- CHICAGO ----------
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" . Journal of the American Chemical Society 132, no. 32 (2010) : 11132-11140.
http://dx.doi.org/10.1021/ja1020487
---------- MLA ----------
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" . Journal of the American Chemical Society, vol. 132, no. 32, 2010, pp. 11132-11140.
http://dx.doi.org/10.1021/ja1020487
---------- VANCOUVER ----------
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. J. Am. Chem. Soc. 2010;132(32):11132-11140.
http://dx.doi.org/10.1021/ja1020487