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A conventional symmetric biosupercapacitor based on rusticyanin modified gold electrodes
Malmö University, Faculty of Health and Society (HS), Department of Biomedical Science (BMV).
Malmö University, Faculty of Health and Society (HS), Department of Biomedical Science (BMV).
Malmö University, Faculty of Health and Society (HS), Department of Biomedical Science (BMV).
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2018 (English)In: Journal of Electroanalytical Chemistry, ISSN 1572-6657, Vol. 816, p. 253-258Article in journal (Refereed) Published
Abstract [en]

Here we report on an entirely new kind of bioelectronic device - a conventional biosupercapacitor, which is built from copper containing redox proteins. Prior to biodevice fabrication, detailed spectroelectrochemical studies of the protein, viz. Acidithiobacillus ferrooxidcats rusticyanin, in solution and in adsorbed state, were performed, including estimation of the redox potential of the T1 site (0.62 V vs. NHE), protein midpoint potential when adsorbed on a self-assembled monolayer (0.34 V vs. NHE), as well as biocapacitance of rusticyanin modified gold electrodes (115 mu F cm(-2)). The symmetrical biosupercapacitor based on two identical gold electrodes modified with rusticyanin is able to capacitively store electricity and deliver electric power accumulated mostly in the form of biopseudocapacitance, when charged and discharged externally. When charged during Just 5 s, the biosupercapacitor with a total capacitance of about 73 mu F cm(-2) provided a maximum of 4 mu A cm(-2) peak current at 0.40 V. The biodevice, which can be charged and discharged at least 50 times without a significant loss of ability to store electric energy, had a low leakage current below 50 nA cm(-2).

Place, publisher, year, edition, pages
Elsevier, 2018. Vol. 816, p. 253-258
Keywords [en]
Blorupercapacitor, Biopseudocapacitance, Direct electron transfer, Double-layer capacitance, Rusticyanin
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:mau:diva-4950DOI: 10.1016/j.jelechem.2018.03.060ISI: 000431156900031Scopus ID: 2-s2.0-85045100634Local ID: 26579OAI: oai:DiVA.org:mau-4950DiVA, id: diva2:1401785
Available from: 2020-02-28 Created: 2020-02-28 Last updated: 2024-04-08Bibliographically approved
In thesis
1. Blue copper proteins as bioelements for bioelectronic devices
Open this publication in new window or tab >>Blue copper proteins as bioelements for bioelectronic devices
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is focused on bioelements for biological electric power sources,specifically, on blue copper proteins with and without an intrinsic biocatalyticactivity, i.e. ability to reduce oxygen directly to water. These proteins, viz. differentlaccases, ceruloplasmin, and rusticyanin, were characterised in detailand employed for the construction of both self-charging and conventional biosupercapacitors.First, similarities and particularities of oxygen electroreductionvs. bioelectroreduction were reviewed. Moreover, being a promising candidatefor the construction of autotolerant implantable biocathodes, the electrochemistryof human ceruloplasmin was revisited. For the first time, a clearbioelectrocatalytic reduction of oxygen on ceruloplasmin modified electrodeswas shown. Second, computational design combined with directed evolutionresulted in a high redox potential mutated laccase, GreeDo, with increased redoxpotential of the T1 site, increased activity towards high redox potentialmediators, as well as enhanced stability. Third, GreeDo was electrochemicallycharacterised in detail. The mutant exhibited higher open circuit potentialvalues and onset potentials for oxygen bioelectroreduction compared to the parental laccase, OB-1. Moreover, the operational stability of GreeDo modifiedgraphite electrodes was found to be more than 2 h in a decidedly acidicelectrolyte, in agreement with the extended operational and storage stabilitiesof the enzyme in acidic solutions. Fourth, multi-cell single-electrolyte glucose/oxygen biodevices with adjustable open-circuit and operating voltages,which are independent on the difference in equilibrium redox potentials of thetwo redox couples, gluconolactone/glucose and oxygen/water, viz. 1.18 V, butdependent on the number of half-cells in the biodevice construction, were designedand tested. The biodevices were made from tubular graphite electrodeswith electropolymerised poly(3,4-ethylenedioxythiophene) modified withTrametes hirsuta laccase and Neurospora crassa cellobiose dehydrogenase as the cathodic and anodic biocatalysts, respectively. Due to the interplay betweenfaradaic and non-faradaic electrochemical processes, as well as betweenionic and electronic conductivities, the open-circuit voltage of the self-chargedbiodevice is extraordinarily high, reaching 3 V, when seven biosupercapacitorsoperating in a common electrolyte were connected in series. Moreover,glucose/oxygen biodevices could be externally discharged at an operatingvoltage exceeding the maximal limiting open-circuit value of 1.24 V for thecomplete glucose oxidation. Last but not least, a conventional biosupercapacitor,i.e. a biodevice lacking self-charging ability, was composed of Acidithiobacillusferrooxidans rusticyanin modified gold electrodes. The complete biodevicesas well as separate electrodes were thoroughly characterised electrochemically.The symmetrical biosupercapacitor based on two identical goldelectrodes modified with rusticyanin is able to capacitively store electricityand deliver electric power, accumulated mostly in the form of biopseudocapacitance,when charged and discharged externally.

Place, publisher, year, edition, pages
Malmö university, 2019. p. 77
Series
Malmö University Health and Society Dissertations, ISSN 1653-5383 ; 2
Keywords
Blue copper protein, Multicopper oxidase, Direct electron transfer, Oxygen bioelectroreduction, Enzymatic fuel cell, Biosupercapacitor
National Category
Medical and Health Sciences
Identifiers
urn:nbn:se:mau:diva-7341 (URN)10.24834/9789178770014 (DOI)28677 (Local ID)9789178770007 (ISBN)9789178770014 (ISBN)28677 (Archive number)28677 (OAI)
Note

Contribution:Paper I. Performed electrochemical investigations of human ceruloplasmin,purified from human blood, on nanostructured graphite electrodes. Took partin literature review, writing of the section 2.3 and preparation of graphicaldata.

Available from: 2020-02-28 Created: 2020-02-28 Last updated: 2022-02-24Bibliographically approved

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Gonzalez-Arribas, ElenaFalk, MagnusAleksejeva, OlgaShleev, Sergey

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