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Mediatorless sugar/oxygen enzymatic fuel cells based on gold nanoparticle-modified electrodes

Wang, Xiaoju; Falk, Magnus; Ortiz, Roberto LU ; Matsumura, Hirotoshi; Bobacka, Johan; Ludwig, Roland; Bergelin, Mikael; Gorton, Lo LU and Shleev, Sergey (2012) In Biosensors & Bioelectronics 31(1). p.219-225
Abstract
We report on the fabrication and characterisation of a gold-nanoparticle (AuNP)-based mediatorless sugar/oxygen biofuel cell (BFC) operating in neutral sugar-containing buffers and human physiological fluids, such as blood and plasma. First, Corynascus thermophilus cellobiose dehydrogenase (CtCDH) and Myrotheciumverrucaria bilirubin oxidase (MvBOx), used as anodic and cathodic bioelements, respectively, were immobilised on gold electrodes modified with 20 nm AuNPs. Detailed characterisation and optimisation of a new CDH/AuNP-based bioanode were performed and the following fundamental parameters were obtained: (i) the redox potential of the haem-containing centre of the enzyme was measured to be 75 mV vs. NHE, (ii) the surface coverage of... (More)
We report on the fabrication and characterisation of a gold-nanoparticle (AuNP)-based mediatorless sugar/oxygen biofuel cell (BFC) operating in neutral sugar-containing buffers and human physiological fluids, such as blood and plasma. First, Corynascus thermophilus cellobiose dehydrogenase (CtCDH) and Myrotheciumverrucaria bilirubin oxidase (MvBOx), used as anodic and cathodic bioelements, respectively, were immobilised on gold electrodes modified with 20 nm AuNPs. Detailed characterisation and optimisation of a new CDH/AuNP-based bioanode were performed and the following fundamental parameters were obtained: (i) the redox potential of the haem-containing centre of the enzyme was measured to be 75 mV vs. NHE, (ii) the surface coverage of CtCDH was found to be 0.65 pmol cm(-2) corresponding to a sub-monolayer coverage of the thiol-modified AuNPs by the enzyme, (iii) a turnover number for CtCDH immobilised on thiol-modified AuNPs was calculated to be ca. 0.5 s(-1), and (iv) the maximal current densities as high as 40 mu A cm(-2) were registered in sugar-containing neutral buffers. Second, both biomodified electrodes, namely the CtCDH/AuNP-based bioanode and the MvBOx/AuNP-based biocathode, were combined into a functional BFC and the designed biodevices were carefully investigated. The following characteristics of the mediator-, separator- and membrane-less, miniature BFC were obtained: in phosphate buffer; an open-circuit voltage of 0.68 V, a maximum power density of 15 mu W cm(-2) at a cell voltage of 0.52 V and in human blood; an open-circuit voltage of 0.65 V. a maximum power density of 3 mu W cm(-2) at a cell voltage of 0.45 V, respectively. The estimated half-lives of the biodevices were found to be >12, <8, and <2h in a sugar-containing buffer, human plasma, and blood, respectively. The basic characteristics of mediatorless sugar/oxygen BFCs were significantly improved compared with previously designed biodevices, because of the usage of three-dimensional AuNP-modified electrodes. (C) 2011 Elsevier B.V. All rights reserved. (Less)
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author
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publishing date
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Contribution to journal
publication status
published
subject
keywords
Enzymatic fuel cells, Direct electron transfer, Gold nanoparticles, Cellobiose dehydrogenase, Bilirubin oxidase
in
Biosensors & Bioelectronics
volume
31
issue
1
pages
219 - 225
publisher
Elsevier
external identifiers
  • wos:000300468400034
  • scopus:84455205563
ISSN
1873-4235
DOI
10.1016/j.bios.2011.10.020
language
English
LU publication?
yes
id
6c3850fc-80a1-4d7f-816c-4f6fb574727c (old id 2403228)
date added to LUP
2012-03-28 13:34:29
date last changed
2017-10-29 04:04:35
@article{6c3850fc-80a1-4d7f-816c-4f6fb574727c,
  abstract     = {We report on the fabrication and characterisation of a gold-nanoparticle (AuNP)-based mediatorless sugar/oxygen biofuel cell (BFC) operating in neutral sugar-containing buffers and human physiological fluids, such as blood and plasma. First, Corynascus thermophilus cellobiose dehydrogenase (CtCDH) and Myrotheciumverrucaria bilirubin oxidase (MvBOx), used as anodic and cathodic bioelements, respectively, were immobilised on gold electrodes modified with 20 nm AuNPs. Detailed characterisation and optimisation of a new CDH/AuNP-based bioanode were performed and the following fundamental parameters were obtained: (i) the redox potential of the haem-containing centre of the enzyme was measured to be 75 mV vs. NHE, (ii) the surface coverage of CtCDH was found to be 0.65 pmol cm(-2) corresponding to a sub-monolayer coverage of the thiol-modified AuNPs by the enzyme, (iii) a turnover number for CtCDH immobilised on thiol-modified AuNPs was calculated to be ca. 0.5 s(-1), and (iv) the maximal current densities as high as 40 mu A cm(-2) were registered in sugar-containing neutral buffers. Second, both biomodified electrodes, namely the CtCDH/AuNP-based bioanode and the MvBOx/AuNP-based biocathode, were combined into a functional BFC and the designed biodevices were carefully investigated. The following characteristics of the mediator-, separator- and membrane-less, miniature BFC were obtained: in phosphate buffer; an open-circuit voltage of 0.68 V, a maximum power density of 15 mu W cm(-2) at a cell voltage of 0.52 V and in human blood; an open-circuit voltage of 0.65 V. a maximum power density of 3 mu W cm(-2) at a cell voltage of 0.45 V, respectively. The estimated half-lives of the biodevices were found to be &gt;12, &lt;8, and &lt;2h in a sugar-containing buffer, human plasma, and blood, respectively. The basic characteristics of mediatorless sugar/oxygen BFCs were significantly improved compared with previously designed biodevices, because of the usage of three-dimensional AuNP-modified electrodes. (C) 2011 Elsevier B.V. All rights reserved.},
  author       = {Wang, Xiaoju and Falk, Magnus and Ortiz, Roberto and Matsumura, Hirotoshi and Bobacka, Johan and Ludwig, Roland and Bergelin, Mikael and Gorton, Lo and Shleev, Sergey},
  issn         = {1873-4235},
  keyword      = {Enzymatic fuel cells,Direct electron transfer,Gold nanoparticles,Cellobiose dehydrogenase,Bilirubin oxidase},
  language     = {eng},
  number       = {1},
  pages        = {219--225},
  publisher    = {Elsevier},
  series       = {Biosensors & Bioelectronics},
  title        = {Mediatorless sugar/oxygen enzymatic fuel cells based on gold nanoparticle-modified electrodes},
  url          = {http://dx.doi.org/10.1016/j.bios.2011.10.020},
  volume       = {31},
  year         = {2012},
}