A glucose/oxygen enzymatic fuel cell based on gold nanoparticles modified graphene screen-printed electrode. Proof-of-concept in human saliva

Paolo Bollella, Giovanni Fusco, Daniela Stevar, Lo Gorton, Roland Ludwig, Su Ma, Harry Boer, Anu Koivula, Cristina Tortolini, Gabriele Favero, Riccarda Antiochia (Corresponding Author), Franco Mazzei (Corresponding Author)

Research output: Contribution to journalArticleScientificpeer-review

19 Citations (Scopus)

Abstract

This paper presents a new direct electron transfer based-miniaturized glucose/oxygen enzymatic fuel cell (EFC) whose operating ability has been tested in real saliva samples. The bioanode and biocathode are a graphene working electrode and a graphite counter electrode localized on the same screen printed electrode (SPE) modified with poly(vinyl alcohol) N-methyl-4(4′-formylstyryl)pyridinium methosulfate acetal (PVA-SbQ)/cellobiose dehydrogenase from Corynascus Thermophilus (CtCDH) C291Y/AuNPs and with Trametes Hirsuta laccase (ThLac)/AuNPs, respectively.
In order to optimize the bioanode, several CDH immobilization procedures were adopted, such as drop-casting, use of Nafion membrane or PVA-SbQ photopolymer. The photopolymer showed the best performance in terms of stability and reliability. As biocathode a partially optimized laccase electrode was employed with the variant that the used nanomaterials allowed to reduce the overpotential of O2/H2O redox reaction catalyzed by Trametes Hirsuta Laccase (ThLac), drop-casted onto the gold nanoparticles (AuNPs) modified SPE.
The performances of bioanode and biocathode were tested separately, initially immobilizing the two enzymes onto separated graphene SPEs. An efficient direct electron transfer was achieved for both elements, obtaining an apparent heterogeneous electron transfer rate constant (ks) of 0.99 ± 0.05 s−1 for CtCDH C291Y and 5.60 ± 0.05 s−1 for ThLac. Both electrodes were then assembled in a two compartment EFC obtaining a maximal power output of 5.16 ± 0.15 μW cm−2 at a cell voltage of 0.58 V and an open circuit voltage (OCV) of 0.74 V. Successively, the bioanode and biocathode were assembled in a non-compartmentalized EFC and a remarkable 50% decrease of the maximum power output at the value of 2.15 ± 0.12 μW cm−2 at cell voltage of 0.48 V and an OCV of 0.62 V at pH 6.5 was registered. In order to reduce the cell dimensions in view of its possible integration in biomedical devices, the bioanode and biocaythode were realized by immobilization of both enzymes onto the same SPE. The so miniaturized EFC delivered a maximal power output of 1.57 ± 0.07 μW cm2 and 1.10 ± 0.12 μW cm−2 with an OCV of 0.58 V and 0.41 V in a 100 μM glucose solution and in human saliva, respectively.
Original languageEnglish
Pages (from-to)921-930
Number of pages10
JournalSensors and Actuators B: Chemical
Volume256
Early online date2017
DOIs
Publication statusPublished - 2018
MoE publication typeA1 Journal article-refereed

Fingerprint

Enzymatic fuel cells
saliva
Graphite
glucose
Gold
Graphene
fuel cells
Glucose
graphene
Laccase
gold
Oxygen
Nanoparticles
nanoparticles
Electrodes
electrodes
oxygen
Open circuit voltage
open circuit voltage
Photopolymers

Keywords

  • AuNPs
  • cellobiose dehydrogenase
  • direct electron transfer
  • enzymatic fuel cells (EFCs)
  • human saliva
  • laccase

Cite this

Bollella, Paolo ; Fusco, Giovanni ; Stevar, Daniela ; Gorton, Lo ; Ludwig, Roland ; Ma, Su ; Boer, Harry ; Koivula, Anu ; Tortolini, Cristina ; Favero, Gabriele ; Antiochia, Riccarda ; Mazzei, Franco. / A glucose/oxygen enzymatic fuel cell based on gold nanoparticles modified graphene screen-printed electrode. Proof-of-concept in human saliva. In: Sensors and Actuators B: Chemical. 2018 ; Vol. 256. pp. 921-930.
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abstract = "This paper presents a new direct electron transfer based-miniaturized glucose/oxygen enzymatic fuel cell (EFC) whose operating ability has been tested in real saliva samples. The bioanode and biocathode are a graphene working electrode and a graphite counter electrode localized on the same screen printed electrode (SPE) modified with poly(vinyl alcohol) N-methyl-4(4′-formylstyryl)pyridinium methosulfate acetal (PVA-SbQ)/cellobiose dehydrogenase from Corynascus Thermophilus (CtCDH) C291Y/AuNPs and with Trametes Hirsuta laccase (ThLac)/AuNPs, respectively.In order to optimize the bioanode, several CDH immobilization procedures were adopted, such as drop-casting, use of Nafion membrane or PVA-SbQ photopolymer. The photopolymer showed the best performance in terms of stability and reliability. As biocathode a partially optimized laccase electrode was employed with the variant that the used nanomaterials allowed to reduce the overpotential of O2/H2O redox reaction catalyzed by Trametes Hirsuta Laccase (ThLac), drop-casted onto the gold nanoparticles (AuNPs) modified SPE.The performances of bioanode and biocathode were tested separately, initially immobilizing the two enzymes onto separated graphene SPEs. An efficient direct electron transfer was achieved for both elements, obtaining an apparent heterogeneous electron transfer rate constant (ks) of 0.99 ± 0.05 s−1 for CtCDH C291Y and 5.60 ± 0.05 s−1 for ThLac. Both electrodes were then assembled in a two compartment EFC obtaining a maximal power output of 5.16 ± 0.15 μW cm−2 at a cell voltage of 0.58 V and an open circuit voltage (OCV) of 0.74 V. Successively, the bioanode and biocathode were assembled in a non-compartmentalized EFC and a remarkable 50{\%} decrease of the maximum power output at the value of 2.15 ± 0.12 μW cm−2 at cell voltage of 0.48 V and an OCV of 0.62 V at pH 6.5 was registered. In order to reduce the cell dimensions in view of its possible integration in biomedical devices, the bioanode and biocaythode were realized by immobilization of both enzymes onto the same SPE. The so miniaturized EFC delivered a maximal power output of 1.57 ± 0.07 μW cm2 and 1.10 ± 0.12 μW cm−2 with an OCV of 0.58 V and 0.41 V in a 100 μM glucose solution and in human saliva, respectively.",
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A glucose/oxygen enzymatic fuel cell based on gold nanoparticles modified graphene screen-printed electrode. Proof-of-concept in human saliva. / Bollella, Paolo; Fusco, Giovanni; Stevar, Daniela; Gorton, Lo; Ludwig, Roland; Ma, Su; Boer, Harry; Koivula, Anu; Tortolini, Cristina; Favero, Gabriele; Antiochia, Riccarda (Corresponding Author); Mazzei, Franco (Corresponding Author).

In: Sensors and Actuators B: Chemical, Vol. 256, 2018, p. 921-930.

Research output: Contribution to journalArticleScientificpeer-review

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T1 - A glucose/oxygen enzymatic fuel cell based on gold nanoparticles modified graphene screen-printed electrode. Proof-of-concept in human saliva

AU - Bollella, Paolo

AU - Fusco, Giovanni

AU - Stevar, Daniela

AU - Gorton, Lo

AU - Ludwig, Roland

AU - Ma, Su

AU - Boer, Harry

AU - Koivula, Anu

AU - Tortolini, Cristina

AU - Favero, Gabriele

AU - Antiochia, Riccarda

AU - Mazzei, Franco

PY - 2018

Y1 - 2018

N2 - This paper presents a new direct electron transfer based-miniaturized glucose/oxygen enzymatic fuel cell (EFC) whose operating ability has been tested in real saliva samples. The bioanode and biocathode are a graphene working electrode and a graphite counter electrode localized on the same screen printed electrode (SPE) modified with poly(vinyl alcohol) N-methyl-4(4′-formylstyryl)pyridinium methosulfate acetal (PVA-SbQ)/cellobiose dehydrogenase from Corynascus Thermophilus (CtCDH) C291Y/AuNPs and with Trametes Hirsuta laccase (ThLac)/AuNPs, respectively.In order to optimize the bioanode, several CDH immobilization procedures were adopted, such as drop-casting, use of Nafion membrane or PVA-SbQ photopolymer. The photopolymer showed the best performance in terms of stability and reliability. As biocathode a partially optimized laccase electrode was employed with the variant that the used nanomaterials allowed to reduce the overpotential of O2/H2O redox reaction catalyzed by Trametes Hirsuta Laccase (ThLac), drop-casted onto the gold nanoparticles (AuNPs) modified SPE.The performances of bioanode and biocathode were tested separately, initially immobilizing the two enzymes onto separated graphene SPEs. An efficient direct electron transfer was achieved for both elements, obtaining an apparent heterogeneous electron transfer rate constant (ks) of 0.99 ± 0.05 s−1 for CtCDH C291Y and 5.60 ± 0.05 s−1 for ThLac. Both electrodes were then assembled in a two compartment EFC obtaining a maximal power output of 5.16 ± 0.15 μW cm−2 at a cell voltage of 0.58 V and an open circuit voltage (OCV) of 0.74 V. Successively, the bioanode and biocathode were assembled in a non-compartmentalized EFC and a remarkable 50% decrease of the maximum power output at the value of 2.15 ± 0.12 μW cm−2 at cell voltage of 0.48 V and an OCV of 0.62 V at pH 6.5 was registered. In order to reduce the cell dimensions in view of its possible integration in biomedical devices, the bioanode and biocaythode were realized by immobilization of both enzymes onto the same SPE. The so miniaturized EFC delivered a maximal power output of 1.57 ± 0.07 μW cm2 and 1.10 ± 0.12 μW cm−2 with an OCV of 0.58 V and 0.41 V in a 100 μM glucose solution and in human saliva, respectively.

AB - This paper presents a new direct electron transfer based-miniaturized glucose/oxygen enzymatic fuel cell (EFC) whose operating ability has been tested in real saliva samples. The bioanode and biocathode are a graphene working electrode and a graphite counter electrode localized on the same screen printed electrode (SPE) modified with poly(vinyl alcohol) N-methyl-4(4′-formylstyryl)pyridinium methosulfate acetal (PVA-SbQ)/cellobiose dehydrogenase from Corynascus Thermophilus (CtCDH) C291Y/AuNPs and with Trametes Hirsuta laccase (ThLac)/AuNPs, respectively.In order to optimize the bioanode, several CDH immobilization procedures were adopted, such as drop-casting, use of Nafion membrane or PVA-SbQ photopolymer. The photopolymer showed the best performance in terms of stability and reliability. As biocathode a partially optimized laccase electrode was employed with the variant that the used nanomaterials allowed to reduce the overpotential of O2/H2O redox reaction catalyzed by Trametes Hirsuta Laccase (ThLac), drop-casted onto the gold nanoparticles (AuNPs) modified SPE.The performances of bioanode and biocathode were tested separately, initially immobilizing the two enzymes onto separated graphene SPEs. An efficient direct electron transfer was achieved for both elements, obtaining an apparent heterogeneous electron transfer rate constant (ks) of 0.99 ± 0.05 s−1 for CtCDH C291Y and 5.60 ± 0.05 s−1 for ThLac. Both electrodes were then assembled in a two compartment EFC obtaining a maximal power output of 5.16 ± 0.15 μW cm−2 at a cell voltage of 0.58 V and an open circuit voltage (OCV) of 0.74 V. Successively, the bioanode and biocathode were assembled in a non-compartmentalized EFC and a remarkable 50% decrease of the maximum power output at the value of 2.15 ± 0.12 μW cm−2 at cell voltage of 0.48 V and an OCV of 0.62 V at pH 6.5 was registered. In order to reduce the cell dimensions in view of its possible integration in biomedical devices, the bioanode and biocaythode were realized by immobilization of both enzymes onto the same SPE. The so miniaturized EFC delivered a maximal power output of 1.57 ± 0.07 μW cm2 and 1.10 ± 0.12 μW cm−2 with an OCV of 0.58 V and 0.41 V in a 100 μM glucose solution and in human saliva, respectively.

KW - AuNPs

KW - cellobiose dehydrogenase

KW - direct electron transfer

KW - enzymatic fuel cells (EFCs)

KW - human saliva

KW - laccase

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