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Nanoscale Optimization of the Direct Electron Transfer Process in Biocathodes Loaded with Multicopper Oxidases

AutorPita, Marcos ; Shleev, Sergey; Lacey, Antonio L. de
Fecha de publicaciónago-2013
CitaciónSeventh International Conference on Quantum, Nano and Micro Technologies (2013)
ResumenMulticopper oxidases (MCO) such as Laccase and Bilirubin Oxidase are one of the best candidates for enzymatic biofuel cell cathodes due to its ability to reduce O2 directly to H2O at high potentials; laccases are also suitable for direct electron transfer when appropriately wired toward different electroactive surfaces such as gold or graphite. However, laccase faces several hindering conditions when taking to many in vivo-like environments, being the most relevant chloride inhibition and the functional pH. Chloride anions are a reversible inhibitor of laccase and are present in most biological fluids. Additionally, the typically acidic pH-optima for laccase performance take any laccase- modified electrode out of range for many natural fluids.
This presentation will show strategies to improve MCOsʼ performance under these non- favoured environments. It has been shown that specific orientation of MCO for DET can reduce this inhibition source when immobilized on a low-density graphite (LDG) electrode and how to extend this immobilization method to gold planar electrodes. We will show the improvement brought to current density and chloride resistance by combining a LDG electrode with gold nanoparticles. The limitations brought by the use of neutral pH can be addressed by generation of a local acidic pH environment. This has been achieved by inserting the MCO electrode in a magnetic ring that allows the deposition of magnetic nanoparticles carrying another enzyme able to acidify the environment. For conceptual purposes we have used glucose oxidase (GOx) to produce a gluconic-acid environment, managing to lower pH 2 units while keeping the bulk pH neutral and therefore allowing laccase to work. Catalase was present for oxygen-regeneration purposes. Development of graphitic-nanostructured electrodes including carbon nanotubes or gold nanoparticles has also been developed, showing a great improvement in the biocathodeʼs performance.
DescripciónTrabajo presentado en la Seventh International Conference on Quantum, Nano and Micro Technologies (ICQNM 2013), celebrada en Barcelona del 25 al 31 de agosto de 2013.
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