Direct electron transfer of trametes hirsuta laccase in a dual-layer architecture of poly(3,4-ethylenedioxythiophene) films

X. Wang, R.-M. Latonen, P. Sjöberg-Eerola, J.-E. Eriksson, J. Bobacka, Harry Boer, M. Bergelin (Corresponding Author)

Research output: Contribution to journalArticleScientificpeer-review

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Abstract

Direct electron transfer (DET) type biocatalysis was accomplished for Trametes hirsuta laccase (ThL) on a glassy carbon (GC) electrode by immobilizing laccase into a well-designed dual-layer architecture of poly(3,4-ethylenedioxythiophene) (PEDOT). PEDOT films were subsequently deposited on a GC electrode via electropolymerization, with NO3− as the counterion for the first accommodation layer and poly(styrene-sulfonate) anions (PSS−) for the second capping layer. The enzyme (ThL) was cast on top of the accommodation layer (PEDOT-NO3), and then the capping layer (PEDOT-PSS) was electrodeposited to entrap ThL between the layers. This enzyme electrode is reported to be able to promote DET between ThL and the GC electrode and catalyze the reduction of O2 into water. The influence of fabrication parameters on the enzyme electrode performance was investigated through chronoamperometric measurements. The investigated parameters included different combinations of PEDOT films, ThL loading, and the thicknesses of both PEDOT layers. As a representative, one optimized dual-layer-architecture enzyme electrode of PEDOT-NO3 (28 mC)/ThL (1.26 U)/PEDOT-PSS (3.5 mC) performed fairly good reproducibility and operational stability. Its pH profile exhibited a bell-shape with an optimal pH in the range of 3.0−3.5. The influences of ionic strength and addition of a nonionic surfactant into the buffer solution on the enzyme electrode performance were also studied to obtain information about the DET mechanism of ThL in the dual-layer architecture. On the basis of the information obtained from different characterizations, π−π interaction between the PSS− ions and the hydrophobic substrate-binding pocket in the vicinity of the T1 Cu site was proposed to result in a favorable location of the conducting polymer chain close to the T1 Cu site and thus facilitate DET of ThL within this particular architecture. The applicability of this approach to various electrode materials is also underlined, which makes it a favorable approach to construct an O2-consuming cathode for biofuel cells.
Original languageEnglish
Pages (from-to)5919-5929
Number of pages11
JournalJournal of Physical Chemistry C
Volume115
Issue number13
DOIs
Publication statusPublished - 2011
MoE publication typeA1 Journal article-refereed

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Enzyme electrodes
Laccase
electron transfer
Glassy carbon
Electrodes
Electrons
enzymes
electrodes
glassy carbon
Biological fuel cells
Electropolymerization
Nonionic surfactants
Conducting polymers
Ionic strength
accommodation
Styrene
Cathodes
Negative ions
Enzymes
Fabrication

Cite this

Wang, X. ; Latonen, R.-M. ; Sjöberg-Eerola, P. ; Eriksson, J.-E. ; Bobacka, J. ; Boer, Harry ; Bergelin, M. / Direct electron transfer of trametes hirsuta laccase in a dual-layer architecture of poly(3,4-ethylenedioxythiophene) films. In: Journal of Physical Chemistry C. 2011 ; Vol. 115, No. 13. pp. 5919-5929.
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abstract = "Direct electron transfer (DET) type biocatalysis was accomplished for Trametes hirsuta laccase (ThL) on a glassy carbon (GC) electrode by immobilizing laccase into a well-designed dual-layer architecture of poly(3,4-ethylenedioxythiophene) (PEDOT). PEDOT films were subsequently deposited on a GC electrode via electropolymerization, with NO3− as the counterion for the first accommodation layer and poly(styrene-sulfonate) anions (PSS−) for the second capping layer. The enzyme (ThL) was cast on top of the accommodation layer (PEDOT-NO3), and then the capping layer (PEDOT-PSS) was electrodeposited to entrap ThL between the layers. This enzyme electrode is reported to be able to promote DET between ThL and the GC electrode and catalyze the reduction of O2 into water. The influence of fabrication parameters on the enzyme electrode performance was investigated through chronoamperometric measurements. The investigated parameters included different combinations of PEDOT films, ThL loading, and the thicknesses of both PEDOT layers. As a representative, one optimized dual-layer-architecture enzyme electrode of PEDOT-NO3 (28 mC)/ThL (1.26 U)/PEDOT-PSS (3.5 mC) performed fairly good reproducibility and operational stability. Its pH profile exhibited a bell-shape with an optimal pH in the range of 3.0−3.5. The influences of ionic strength and addition of a nonionic surfactant into the buffer solution on the enzyme electrode performance were also studied to obtain information about the DET mechanism of ThL in the dual-layer architecture. On the basis of the information obtained from different characterizations, π−π interaction between the PSS− ions and the hydrophobic substrate-binding pocket in the vicinity of the T1 Cu site was proposed to result in a favorable location of the conducting polymer chain close to the T1 Cu site and thus facilitate DET of ThL within this particular architecture. The applicability of this approach to various electrode materials is also underlined, which makes it a favorable approach to construct an O2-consuming cathode for biofuel cells.",
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Direct electron transfer of trametes hirsuta laccase in a dual-layer architecture of poly(3,4-ethylenedioxythiophene) films. / Wang, X.; Latonen, R.-M.; Sjöberg-Eerola, P.; Eriksson, J.-E.; Bobacka, J.; Boer, Harry; Bergelin, M. (Corresponding Author).

In: Journal of Physical Chemistry C, Vol. 115, No. 13, 2011, p. 5919-5929.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - Direct electron transfer of trametes hirsuta laccase in a dual-layer architecture of poly(3,4-ethylenedioxythiophene) films

AU - Wang, X.

AU - Latonen, R.-M.

AU - Sjöberg-Eerola, P.

AU - Eriksson, J.-E.

AU - Bobacka, J.

AU - Boer, Harry

AU - Bergelin, M.

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N2 - Direct electron transfer (DET) type biocatalysis was accomplished for Trametes hirsuta laccase (ThL) on a glassy carbon (GC) electrode by immobilizing laccase into a well-designed dual-layer architecture of poly(3,4-ethylenedioxythiophene) (PEDOT). PEDOT films were subsequently deposited on a GC electrode via electropolymerization, with NO3− as the counterion for the first accommodation layer and poly(styrene-sulfonate) anions (PSS−) for the second capping layer. The enzyme (ThL) was cast on top of the accommodation layer (PEDOT-NO3), and then the capping layer (PEDOT-PSS) was electrodeposited to entrap ThL between the layers. This enzyme electrode is reported to be able to promote DET between ThL and the GC electrode and catalyze the reduction of O2 into water. The influence of fabrication parameters on the enzyme electrode performance was investigated through chronoamperometric measurements. The investigated parameters included different combinations of PEDOT films, ThL loading, and the thicknesses of both PEDOT layers. As a representative, one optimized dual-layer-architecture enzyme electrode of PEDOT-NO3 (28 mC)/ThL (1.26 U)/PEDOT-PSS (3.5 mC) performed fairly good reproducibility and operational stability. Its pH profile exhibited a bell-shape with an optimal pH in the range of 3.0−3.5. The influences of ionic strength and addition of a nonionic surfactant into the buffer solution on the enzyme electrode performance were also studied to obtain information about the DET mechanism of ThL in the dual-layer architecture. On the basis of the information obtained from different characterizations, π−π interaction between the PSS− ions and the hydrophobic substrate-binding pocket in the vicinity of the T1 Cu site was proposed to result in a favorable location of the conducting polymer chain close to the T1 Cu site and thus facilitate DET of ThL within this particular architecture. The applicability of this approach to various electrode materials is also underlined, which makes it a favorable approach to construct an O2-consuming cathode for biofuel cells.

AB - Direct electron transfer (DET) type biocatalysis was accomplished for Trametes hirsuta laccase (ThL) on a glassy carbon (GC) electrode by immobilizing laccase into a well-designed dual-layer architecture of poly(3,4-ethylenedioxythiophene) (PEDOT). PEDOT films were subsequently deposited on a GC electrode via electropolymerization, with NO3− as the counterion for the first accommodation layer and poly(styrene-sulfonate) anions (PSS−) for the second capping layer. The enzyme (ThL) was cast on top of the accommodation layer (PEDOT-NO3), and then the capping layer (PEDOT-PSS) was electrodeposited to entrap ThL between the layers. This enzyme electrode is reported to be able to promote DET between ThL and the GC electrode and catalyze the reduction of O2 into water. The influence of fabrication parameters on the enzyme electrode performance was investigated through chronoamperometric measurements. The investigated parameters included different combinations of PEDOT films, ThL loading, and the thicknesses of both PEDOT layers. As a representative, one optimized dual-layer-architecture enzyme electrode of PEDOT-NO3 (28 mC)/ThL (1.26 U)/PEDOT-PSS (3.5 mC) performed fairly good reproducibility and operational stability. Its pH profile exhibited a bell-shape with an optimal pH in the range of 3.0−3.5. The influences of ionic strength and addition of a nonionic surfactant into the buffer solution on the enzyme electrode performance were also studied to obtain information about the DET mechanism of ThL in the dual-layer architecture. On the basis of the information obtained from different characterizations, π−π interaction between the PSS− ions and the hydrophobic substrate-binding pocket in the vicinity of the T1 Cu site was proposed to result in a favorable location of the conducting polymer chain close to the T1 Cu site and thus facilitate DET of ThL within this particular architecture. The applicability of this approach to various electrode materials is also underlined, which makes it a favorable approach to construct an O2-consuming cathode for biofuel cells.

U2 - 10.1021/jp1080065

DO - 10.1021/jp1080065

M3 - Article

VL - 115

SP - 5919

EP - 5929

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 13

ER -