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1.
Nanoscale ; 7(24): 10641-7, 2015 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-26024212

RESUMO

Glucose oxidase (GOx) is immobilized on ZnO nanoparticle-modified electrodes. The immobilized glucose oxidase shows efficient mediated electron transfer with ZnO nanoparticles to which the ferrocenyl moiety is π-stacked into a supramolecular architecture. The constructed ZnO-Fc/CNT modified electrode exhibits high ferrocene surface coverage, preventing any leakage of the π-stacked ferrocene from the newly described ZnO hybrid nanoparticles. The use of the new architecture of ZnO supported electron mediators to shuttle electrons from the redox centre of the enzyme to the surface of the working electrode can effectively bring about successful glucose oxidation. These modified electrodes evaluated as a highly efficient architecture provide a catalytic current for glucose oxidation and are integrated in a specially designed glucose/air fuel cell prototype using a conventional platinum-carbon (Pt/C) cathode at physiological pH (7.0). The obtained architecture leads to a peak power density of 53 µW cm(-2) at 300 mV for the Nafion® based biofuel cell under "air breathing" conditions at room temperature.


Assuntos
Fontes de Energia Bioelétrica , Eletrodos , Glucose Oxidase/química , Glucose/química , Nanotubos de Carbono/química , Óxido de Zinco/química , Transferência de Energia , Enzimas Imobilizadas/química , Desenho de Equipamento , Análise de Falha de Equipamento , Nanoconjugados/química , Nanofios/química
2.
J Am Chem Soc ; 134(34): 14078-85, 2012 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-22816654

RESUMO

This paper details the electrochemical investigation of a deuteroporphyrin dimethylester (DPDE) rhodium(III) ((DPDE)Rh(III)) complex, immobilized within a MWCNT/Nafion electrode, and its integration into a molecular catalysis-based glucose fuel cell. The domains of present (DPDE)Rh(I), (DPDE)Rh-H, (DPDE)Rh(II), and (DPDE)Rh(III) were characterized by surface electrochemistry performed at a broad pH range. The Pourbaix diagrams (plots of E(1/2) vs pH) support the stability of (DPDE)Rh(II) at intermediate pH and the predominance of the two-electron redox system (DPDE)Rh(I)/(DPDE)Rh(III) at both low and high pH. This two-electron system is especially involved in the electrocatalytic oxidation of alcohols and was applied to the glucose oxidation. The catalytic oxidation mechanism exhibits an oxidative deactivation coupled with a reductive reactivation mechanism, which has previously been observed for redox enzymes but not yet for a metal-based molecular catalyst. The MWCNT/(DPDE)Rh(III) electrode was finally integrated in a novel design of an alkaline glucose/O(2) fuel cell with a MWCNT/phthalocyanin cobalt(II) (CoPc) electrode for the oxygen reduction reaction. This nonenzymatic molecular catalysis-based glucose fuel cell exhibits a power density of P(max) = 0.182 mW cm(-2) at 0.22 V and an open circuit voltage (OCV) of 0.64 V.

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