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Comparison of bioelectrocatalysis at Trichaptum abietinum and Trametes hirsuta laccase modified electrodes
Malmö högskola, Faculty of Health and Society (HS), Department of Biomedical Science (BMV).
Malmö högskola, Faculty of Health and Society (HS), Department of Biomedical Science (BMV).ORCID iD: 0000-0001-6421-2158
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2014 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 130, p. 141-147Article in journal (Refereed) Published
Abstract [en]

Bioelectrocatalytic reduction of oxygen to water at electrodes modified with gold nanoparticles and a new laccase from Trichaptum abietinum (TaLc) was studied. The bioelectrocatalytic current was found to be much higher at TaLc modified electrodes than at similarly prepared electrodes modified with a broadly used laccase from Trametes hirsuta (ThLc). To explain this difference the bioelectrocatalysis was described in terms of kinetic rate constants based on simultaneous cyclic voltammetry and quartz crystal microbalance measurements. From analysis of the rate constants both laccases appeared to possess similar rates (k(0)) of direct electron transfer. However, the enzyme turnover (k(cat)) was about three-fold higher for gold nanoparticle bound TaLc than for ThLc, calculated using surface concentration of enzyme established by QCM-D. Near reversible potential-induced reorientation of adsorbed proteins was observed by surface enhanced Raman spectroscopy. (C) 2014 Elsevier Ltd. All rights reserved.

Place, publisher, year, edition, pages
Elsevier, 2014. Vol. 130, p. 141-147
Keywords [en]
Electron transfer, Bioelectrocatalysis, Oxygen reduction, Gold nanoparticle, Laccase
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:mau:diva-15259DOI: 10.1016/j.electacta.2014.03.014ISI: 000336880700018Scopus ID: 2-s2.0-84897428617Local ID: 18090OAI: oai:DiVA.org:mau-15259DiVA, id: diva2:1418780
Available from: 2020-03-30 Created: 2020-03-30 Last updated: 2024-02-05Bibliographically approved
In thesis
1. Design and characterization of direct electron transfer based biofuel cells including tests in cell cultures
Open this publication in new window or tab >>Design and characterization of direct electron transfer based biofuel cells including tests in cell cultures
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Enzymatic fuel cells (EFCs) are bioelectronic devices based on redox enzymes, which convert chemical energy into electrical energy via biochemical reactions. A major difficulty to overcome is to successfully connect (using e.g., immobilization) the enzymes to the electrode surface. Since the immobilization process often stabilizes the enzyme, the electrode surface and the enzyme/electrode interface is of utmost importance for both the efficiency and stability of the EFC. In this work several different means of establishing the enzyme/electrode connection have been investigated.In order to construct a device that utilizes direct electron transfer the electrode surfaces were modified with nanostructures and, in some designs, self-assembled monolayers of thiols. The performance of the electrodes was evaluated by electrochemical methods, including potential sweeps and chronopotentiometry. Catalytic constants could be calculated mathematically by combining electrochemical methods with surface characterization methods, such as quartz crystal microbalance with dissipation and ellipsometry. All the fuel cells covered by this thesis are based on direct electron transfer processes. All designs also oxidize carbohydrates and reduce oxygen using cellobiose dehydrogenase and multi-copper oxidase, respectively.Our results revealed that the use of particular thiol had the capability to electrically connect cellobiose dehydrogenase to the electrode, equalling the commonly used two-thiol system. Both designs reached similar current densities, Le., about 20 jiA cm 2 with 5 mM lactose and the enzyme immobilized on thiolated gold nanoparticles (AuNPs). Both Bilirubin oxidase and Trichaptum abietinum Laccase could be directly immobilized on gold nanoparticles and current densities of up to 180 pA cm 2 were achieved. The 9- fold difference in currents with BOx and CDH reveals that the bioanode in this system requires more improvement to match the biocathode in performance. Upon doser inspection of the biointerface as regards the bioanode, it was concluded that a positive charge on the thiol was needed to create a direct (electric) contact between CDH and the electrode surface. Furthermore, the catalytic currents were nearly halved when the charged groups on the thiol were further modified with methyl groups.Biocompatibility of an implantable EFC design was evaluated using cell cultures of mammal cells, which was the first study of its kind. Toxicology tests revealed toxic by-products from the bioanode previously not reported in EFCs implanted in animals. The currents of the EFC was reduced by about half in cell culturing medium (10 1.1A cm') compared to PBS solutions, and was even more drastically reduced upon direct contact with fibroblast cells (1 jiA cm').

Place, publisher, year, edition, pages
Malmö university, Faculty of Health and Society, 2014. p. 73
Series
Malmö University Health and Society Dissertations, ISSN 1653-5383 ; 4
Keywords
biofuel cell, enzymatic fuel cell, direct electron transfer, cellobiose dehydrogenase, biocompatibility, enzyme kinetics, cell culture
National Category
Natural Sciences
Identifiers
urn:nbn:se:mau:diva-7317 (URN)17335 (Local ID)978-91-7104-611-6 (ISBN)978-91-7104-612-3 (ISBN)17335 (Archive number)17335 (OAI)
Note

Paper III in dissertation as manuscript with title "Electroactive biomaterial based on enzymatic catalysis and physical factors affecting its performance"

Available from: 2020-02-28 Created: 2020-02-28 Last updated: 2024-01-17Bibliographically approved

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Shleev, SergeyArnebrant, ThomasRuzgas, Tautgirdas

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