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Highly Sensitive Membraneless Fructose Biosensor Based on Fructose Dehydrogenase Immobilized onto Aryl Thiol Modified Highly Porous Gold Electrode : Characterization and Application in Food Samples

Bollella, Paolo ; Hibino, Yuya ; Kano, Kenji ; Gorton, Lo LU and Antiochia, Riccarda (2018) In Analytical Chemistry 90(20). p.12131-12136
Abstract

In this paper we present a new method to electrodeposit highly porous gold (h-PG) onto a polycrystalline solid gold electrode without any template. The electrodeposition is carried out by first cycling the electrode potential between +0.8 and 0 V in 10 mM HAuCl4 with 2.5 M NH4Cl and then applying a negative potential for the production of hydrogen bubbles at the electrode surface. After that the modified electrode was characterized in sulfuric acid to estimate the real surface area (Areal) to be close to 24 cm2, which is roughly 300 times higher compared to the bare gold electrodes (0.08 cm2). The electrode was further incubated overnight with three different thiols... (More)

In this paper we present a new method to electrodeposit highly porous gold (h-PG) onto a polycrystalline solid gold electrode without any template. The electrodeposition is carried out by first cycling the electrode potential between +0.8 and 0 V in 10 mM HAuCl4 with 2.5 M NH4Cl and then applying a negative potential for the production of hydrogen bubbles at the electrode surface. After that the modified electrode was characterized in sulfuric acid to estimate the real surface area (Areal) to be close to 24 cm2, which is roughly 300 times higher compared to the bare gold electrodes (0.08 cm2). The electrode was further incubated overnight with three different thiols (4-mercaptobenzoic acid (4-MBA), 4-mercaptophenol (4-MPh), and 4-aminothiophenol (4-APh)) in order to produce differently charged self-assembled monolayers (SAMs) on the electrode surface. Finally a fructose dehydrogenase (FDH) solution was drop-cast onto the electrodes. All the modified electrodes were investigated by cyclic voltammetry both under nonturnover and turnover conditions. The FDH/4-MPh/h-PG exhibited two couples of redox peaks for the heme c1 and heme c2 of the cytochrome domain of FDH and as well as a well pronounced catalytic current density (about 1000 μA cm-2 in the presence of 10 mM fructose) due to the presence of -OH groups on the electrode surface, which stabilize and orientate the enzyme layer on the electrode surface. The FDH/4-MPh/h-PG based electrode showed the best analytical performance with an excellent stability (90% retained activity over 90 days), a detection limit of 0.3 μM fructose, a linear range between 0.05 and 5 mM, and a sensitivity of 175 ± 15 μA cm-2 mM-1. These properties were favorably compared with other fructose biosensors reported in the literature. The biosensor was successively tested to quantify the fructose content in food and beverage samples. No significant interference present in the sample matrixes was observed.

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author
; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Analytical Chemistry
volume
90
issue
20
pages
6 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85053307946
  • pmid:30148350
ISSN
0003-2700
DOI
10.1021/acs.analchem.8b03093
language
English
LU publication?
yes
id
2d8d270c-5f5f-46c2-a08d-313389af6238
date added to LUP
2018-10-26 07:58:14
date last changed
2024-06-10 20:56:58
@article{2d8d270c-5f5f-46c2-a08d-313389af6238,
  abstract     = {{<p>In this paper we present a new method to electrodeposit highly porous gold (h-PG) onto a polycrystalline solid gold electrode without any template. The electrodeposition is carried out by first cycling the electrode potential between +0.8 and 0 V in 10 mM HAuCl<sub>4</sub> with 2.5 M NH<sub>4</sub>Cl and then applying a negative potential for the production of hydrogen bubbles at the electrode surface. After that the modified electrode was characterized in sulfuric acid to estimate the real surface area (A<sub>real</sub>) to be close to 24 cm<sup>2</sup>, which is roughly 300 times higher compared to the bare gold electrodes (0.08 cm<sup>2</sup>). The electrode was further incubated overnight with three different thiols (4-mercaptobenzoic acid (4-MBA), 4-mercaptophenol (4-MPh), and 4-aminothiophenol (4-APh)) in order to produce differently charged self-assembled monolayers (SAMs) on the electrode surface. Finally a fructose dehydrogenase (FDH) solution was drop-cast onto the electrodes. All the modified electrodes were investigated by cyclic voltammetry both under nonturnover and turnover conditions. The FDH/4-MPh/h-PG exhibited two couples of redox peaks for the heme c<sub>1</sub> and heme c<sub>2</sub> of the cytochrome domain of FDH and as well as a well pronounced catalytic current density (about 1000 μA cm<sup>-2</sup> in the presence of 10 mM fructose) due to the presence of -OH groups on the electrode surface, which stabilize and orientate the enzyme layer on the electrode surface. The FDH/4-MPh/h-PG based electrode showed the best analytical performance with an excellent stability (90% retained activity over 90 days), a detection limit of 0.3 μM fructose, a linear range between 0.05 and 5 mM, and a sensitivity of 175 ± 15 μA cm<sup>-2</sup> mM<sup>-1</sup>. These properties were favorably compared with other fructose biosensors reported in the literature. The biosensor was successively tested to quantify the fructose content in food and beverage samples. No significant interference present in the sample matrixes was observed.</p>}},
  author       = {{Bollella, Paolo and Hibino, Yuya and Kano, Kenji and Gorton, Lo and Antiochia, Riccarda}},
  issn         = {{0003-2700}},
  language     = {{eng}},
  month        = {{10}},
  number       = {{20}},
  pages        = {{12131--12136}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Analytical Chemistry}},
  title        = {{Highly Sensitive Membraneless Fructose Biosensor Based on Fructose Dehydrogenase Immobilized onto Aryl Thiol Modified Highly Porous Gold Electrode : Characterization and Application in Food Samples}},
  url          = {{http://dx.doi.org/10.1021/acs.analchem.8b03093}},
  doi          = {{10.1021/acs.analchem.8b03093}},
  volume       = {{90}},
  year         = {{2018}},
}