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  • 1.
    Sankoh, Supannee
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering. Prince Songkla University, Thailand.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Sekretareva, Alina
    Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Stanford University, CA 94305 USA.
    Thavarungkul, Panote
    Prince Songkla University, Thailand.
    Kanatharana, Proespichaya
    Prince Songkla University, Thailand.
    Mak, Wing Cheung
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Colloid electrochemistry of conducting polymer: towards potential-induced in-situ drug release2017In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 228, p. 407-412Article in journal (Refereed)
    Abstract [en]

    Over the past decades, controlled drug delivery system remains as one of the most important area in medicine for various diseases. We have developed a new electrochemically controlled drug release system by combining colloid electrochemistry and electro-responsive microcapsules. The pulsed electrode potential modulation led to the appearance of two processes available for the time-resolved registration in colloid microenvironment: change of the electronic charge of microparticles (from 0.5 ms to 0.1 s) followed by the drug release associated with ionic equilibration (1-10 s). The dynamic electrochemical measurements allow the distinction of drug release associated With ionic relaxation and the change of electronic charge of conducting polymer colloid microparticles. The amount of released drug (methylene blue) could be controlled by modulating the applied potential. Our study demonstrated a surface-potential driven controlled drug release of dispersion of conducting polymer carrier at the electrode interfaces, while the bulk colloids dispersion away from the electrode remains as a reservoir to improve the efficiency of localized drug release. The developed new methodology creates a model platform for the investigations of surface potential-induced in-situ electrochemical drug release mechanism. (C) 2017 Elsevier Ltd. All rights reserved.

  • 2.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Stanford University, CA 94305 USA.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Correspondence on "Can Nanoimpacts Detect Single-Enzyme Activity? Theoretical Considerations and an Experimental Study of Catalase Impacts"2017In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 7, no 5, p. 3591-3593Article in journal (Other academic)
    Abstract [en]

    n/a

  • 3.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Screen printed microband array based biosensor for water monitoring2015In: The Frumkin Symposium, 2015Conference paper (Refereed)
  • 4.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Uppsala Univ, Sweden.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Evaluation of the Electrochemically Active Surface Area of Microelectrodes by Capacitive and Faradaic Currents2019In: CHEMELECTROCHEM, ISSN 2196-0216, Vol. 6, no 17, p. 4411-4417Article in journal (Refereed)
    Abstract [en]

    Two experimental methods to estimate the electrochemically active surface area (EASA) of microelectrodes are investigated. One method is based on electrocapacitive measurements and depends significantly on the surface roughness as well as on other parameters. The other method is based on faradaic current measurements and depends on the geometric surface area. The experimental results are supplemented with numerical modeling of electrodes with different surface roughness. A systematic study reveals a strong influence of the scale and arrangement of the surface roughness, the measurement potential and the electrolyte concentration on the EASA of microelectrodes estimated from the electrocapacitive measurements. The results show that electrocapacitive measurements should not be used to estimate the faradaic EASA of microelectrodes with a non-negligible surface roughness.

  • 5.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony P.F.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Total phenol analysis of water using a laccase-based microsensor array2015In: Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society. 14-18 June, 2015. Malmö, Sweden, Lausanne: Bioelectrochemical Society , 2015, p. 155-155Conference paper (Other academic)
    Abstract [en]

    The monitoring of phenolic compounds in raw waters and wastewaters is of great importance for environmental control. Use of biosensors for rapid, specific and simple detection of phenolic compounds is a promising approach. A number of biosensors have been developed for phenol detection. A general drawback of previously reported biosensors is their insufficient detection limits for phenols in water samples. One way to improve the detection limit is by the use of microelectrodes.

    Microband design of the microelectrodes combines convergent mass transport due to the microscale width and high output currents due to the macroscopic length. Among the various techniques available for microband electrode fabrication, we have chosen screen-printing which is a cost-effective production method.

    In this study, we report on the development of a laccase-based microscale biosensor operating under a convergent diffusion regime. Screen-printing followed by simple cutting was utilized for the fabrication of graphite microbands as a platform for further covalent immobilization of laccase. Numerical simulations, utilizing the finite element method with periodic boundary conditions, were used for modeling the voltammetric response of the developed microband electrodes. Anodization followed by covalent immobilization was used for the electrode modification with laccase. Direct and mediated laccase bioelectrocatalytic oxidation of phenols was studied on macro- and microscale graphite electrodes. Significant enhancement of the analytical performance was achieved by the establishment of convergent diffusion in the microscale sensor. Finally, the developed microsensor was utilized to monitor phenolic compounds in real waste water.

  • 6.
    Sekretaryova, Alina
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Facilitating electron transfer in bioelectrocatalytic systems2016Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Bioelectrocatalytic systems are based on biological entities, such as enzymes, whole cells, parts of cells or tissues, which catalyse electrochemical processes that involve the interaction between chemical change and electrical energy. In all cases, biocatalysis is implemented by enzymes, isolated or residing inside cells or part of cells. Electron transfer (ET) phenomena, within the protein molecules and between biological redox systems and electronics, enable the development of various bioelectrocatalytic systems, which can be used both for fundamental investigations of enzymatic biological processes by electrochemical methods and for applied purposes, such as power generation, bioremediation, chemical synthesis and biosensing.

    Electrical communication between the biocatalyst’s redox centre and an electrode is essential for the functioning of the system. This can be established using two main mechanisms: indirect ET and direct ET. The efficiency of the ET influences important parameters such as the turnover rate of the biocatalyst, the generated current density and partially the stability of the system, which in their turn determine response time, sensitivity, detection limit and operational stability of biosensing devices or the power densities and current output of biofuel cells, and hence should be carefully considered when designing bioelectrocatalytic systems.

    This thesis focuses on approaches that facilitate ET in bioelectrocatalytic systems based on indirect and direct ET mechanisms. Both fundamental aspects of ET in bioelectrocatalytic systems and applications of such systems for biosensing and power generation are considered. First, a new hydrophobic mediator for oxidases – unsubstituted phenothiazine and its improved ET properties in comparison with commonly used mediators are discussed. Application of the mediator in electrochemical biosensors is demonstrated by glucose, lactate and cholesterol sensing. Utilisation of mediated biocatalytic cholesterol oxidation, as the anodic reaction for the construction of a biofuel cell acting as a power supply and an analytical device at the same time, is investigated to deliver a selfpowered biosensor. Also the enhancement of mediated bioelectrocatalysis by employment of microelectrodes as a transducer is examined. The effect of surface roughness on the current response of the microelectrodes under conditions of convergent diffusion is considered. The applicability of the laccase-based system for total phenol analysis of weakly supported water is demonstrated. Finally, a new electrochemical approach derived from collision-based electrochemistry applicable for examination of the ET process of a single enzyme molecule is described.

    All together, the results presented in this thesis contribute to the solution of the ‘electronic coupling problem’, arising when interfacing biomolecules with electronics and limiting the performance of bioelectrocatalytic systems in specific applications. The developed methods to facilitate ET will hopefully promote future biosensing devices and biofuel cells. I believe the new approach for investigation of ET processes at a single enzyme molecule will complement existing single molecule techniques, giving further insights into enzymatic ET mechanisms at the molecular level and filling the gap between fundamental understanding of biocatalytic processes and their potential for bioenergy production.

    List of papers
    1. Bioelectrocatalytic systems for health applications
    Open this publication in new window or tab >>Bioelectrocatalytic systems for health applications
    2016 (English)In: Biotechnology Advances, ISSN 0734-9750, E-ISSN 1873-1899, Vol. 34, no 3, p. 177-197Article, review/survey (Refereed) Published
    Abstract [en]

    We present a brief overview of bioelectrocatalytic devices for in vitro health applications, including food safety and environmental analysis, focusing on microelectrode- and microfluidic-based biosensors, paper-based point-of-care devices and wearable biosensors. The main hurdles and future perspectives are discussed. We then consider the role of electron transfer between a biocatalyst and an electrode in biosensor design. Brief descriptions of indirect, direct and mediated mechanisms are given. The principal strategies, as well as recent developments for modulation of electron transfer in biocatalytic systems are summarised. In conclusion, we highlight some of the challenges associated with improving these redox systems.

    Place, publisher, year, edition, pages
    Elsevier, 2016
    Keywords
    Direct electron transfer; Mediated electron transfer; Immobilisation; Microbiosensor; Nanobiosensor; Paper-based biosensor; Wearable biosensor; Self-powered biosensor
    National Category
    Bioinformatics and Systems Biology
    Identifiers
    urn:nbn:se:liu:diva-123688 (URN)10.1016/j.biotechadv.2015.12.005 (DOI)000375500700004 ()26724183 (PubMedID)
    Available from: 2016-01-08 Created: 2016-01-08 Last updated: 2017-12-01Bibliographically approved
    2. Reagentless Biosensor Based on Glucose Oxidase Wired by the Mediator Freely Diffusing in Enzyme Containing Membrane
    Open this publication in new window or tab >>Reagentless Biosensor Based on Glucose Oxidase Wired by the Mediator Freely Diffusing in Enzyme Containing Membrane
    Show others...
    2012 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 84, no 3, p. 1220-1223Article in journal (Refereed) Published
    Abstract [en]

    Wiring glucose oxidase in the membrane with an immobilized mediator is possible due to the diffusion ability of the latter, if the enzyme containing membrane is formed according to the proposed protocol, including exposing proteins to water–organic mixtures with the high content of organic solvent. In the course of the study, the new glucose oxidase mediator, unsubstituted phenothiazine, was discovered. The diffusion coefficient of the mediator in the resulting membrane is independent of the presence of enzyme. The cyclic voltammograms of the enzyme electrode after appearance of the only glucose in solution obtain a well-defined catalytic shape, which is normally observed for both the enzyme and the mediator in solution. Analytical performances of the resulting biosensor are comparable to the advanced second generation ones, which, however, require covalent linking of the mediator either to the membrane forming polymer or to the enzyme. Even without such covalent linking, the reported biosensor is characterized by an appropriate long-term operational stability allowing reagentless sensing.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2012
    National Category
    Analytical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-112343 (URN)10.1021/ac203056m (DOI)22206508 (PubMedID)
    Available from: 2014-11-24 Created: 2014-11-24 Last updated: 2017-12-05Bibliographically approved
    3. Unsubstituted phenothiazine as a superior water-insoluble mediator for oxidases
    Open this publication in new window or tab >>Unsubstituted phenothiazine as a superior water-insoluble mediator for oxidases
    Show others...
    2014 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 53, p. 275-282Article in journal (Refereed) Published
    Abstract [en]

    The mediation of oxidases glucose oxidase (GOx), lactate oxidase (LOx) and cholesterol oxidase (ChOx) by a new electron shuttling mediator, unsubstituted phenothiazine (PTZ), was studied. Cyclic voltammetry and rotating-disk electrode measurements in nonaqueous media were used to determine the diffusion characteristics of the mediator and the kinetics of its reaction with GOx, giving a second-order rate constant of 7.6×103–2.1×104 M−1 s−1 for water–acetonitrile solutions containing 5–15% water. These values are in the range reported for commonly used azine-type mediators, indicating that PTZ is able to function as an efficient mediator. PTZ and GOx, LOx and ChOx were successfully co-immobilised in sol–gel membrane on a screen-printed electrode to construct glucose, lactate and cholesterol biosensors, respectively, which were then optimised in terms of stability and sensitivity. The electrocatalytic oxidation responses showed a dependence on substrate concentration ranging from 0.6 to 32 mM for glucose, from 19 to 565 mM for lactate and from 0.015 to 1.0 mM for cholesterol detection. Oxidation of substrates on the surface of electrodes modified with PTZ and enzyme membrane was investigated with double-step chronoamperometry and the results showed that the PTZ displays excellent electrochemical catalytic activities even when immobilised on the surface of the electrode.

    Place, publisher, year, edition, pages
    Elsevier, 2014
    Keywords
    Phenothiazine; Electron transfer mediator; Enzyme biosensor; Glucose oxidase; Lactate oxidase; Cholesterol oxidase
    National Category
    Analytical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-100391 (URN)10.1016/j.bios.2013.09.071 (DOI)000329881100044 ()
    Available from: 2013-11-05 Created: 2013-11-05 Last updated: 2017-12-06Bibliographically approved
    4. Cholesterol Self-Powered Biosensor
    Open this publication in new window or tab >>Cholesterol Self-Powered Biosensor
    Show others...
    2014 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 86, no 19, p. 9540-9547Article in journal (Refereed) Published
    Abstract [en]

    Monitoring the cholesterol level is of great importance, especially for people with high risk of developing heart disease. Here we report on reagentless cholesterol detection in human plasma with a novel single-enzyme, membrane-free, self-powered biosensor, in which both cathodic and anodic bioelectrocatalytic reactions are powered by the same substrate. Cholesterol oxidase was immobilized in a sol-gel matrix on both the cathode and the anode. Hydrogen peroxide, a product of the enzymatic conversion of cholesterol, was electrocatalytically reduced, by the use of Prussian blue, at the cathode. In parallel, cholesterol oxidation catalyzed by mediated cholesterol oxidase occurred at the anode. The analytical performance was assessed for both electrode systems separately. The combination of the two electrodes, formed on high surface-area carbon cloth electrodes, resulted in a self-powered biosensor with enhanced sensitivity (26.0 mA M-1 cm(-2)), compared to either of the two individual electrodes, and a dynamic range up to 4.1 mM cholesterol. Reagentless cholesterol detection with both electrochemical systems and with the self-powered biosensor was performed and the results were compared with the standard method of colorimetric cholesterol quantification.

    Place, publisher, year, edition, pages
    American Chemical Society, 2014
    National Category
    Physical Sciences Biological Sciences
    Identifiers
    urn:nbn:se:liu:diva-112176 (URN)10.1021/ac501699p (DOI)000343017100031 ()25164485 (PubMedID)
    Note

    Funding Agencies|Swedish research council Formas; research centre Security Link; Swedish Institute

    Available from: 2014-11-18 Created: 2014-11-18 Last updated: 2017-12-05
    5. Arrays of Screen-Printed Graphite Microband Electrodes as a Versatile Electroanalysis Platform
    Open this publication in new window or tab >>Arrays of Screen-Printed Graphite Microband Electrodes as a Versatile Electroanalysis Platform
    Show others...
    2014 (English)In: ChemElectroChem, ISSN 2196-0216, Vol. 1, no 4, p. 755-762Article in journal (Refereed) Published
    Abstract [en]

    Arrays of microband electrodes were developed by screen printing followed by cutting, which enabled the realization of microband arrays at the cut edge. The microband arrays of different designs were characterized by physical and electro-chemical methods. In both cases, the methods showed that the microband width was around 5 mm. Semi-steady-state cyclic voltammetry responses were observed for redox probes, and chronocoulometric measurements showed the establishment of convergent diffusion regimes characterized by current densities similar to those of a single microelectrode. The analytical performance of the electrode system and its versatility were illustrated with two electrochemical assays: detection of ascorbic acid through direct oxidation and a mediated glucose biosensor fabricated by dip coating. Due to convergent mass transport, both systems showed an enhancement in their analytical characteristics. The developed approach can be adapted to automated electrode recovery.

    Place, publisher, year, edition, pages
    Wiley, 2014
    Keywords
    graphite screen printing; microarrays; microband; sensors; voltammetry
    National Category
    Physical Sciences Chemical Sciences
    Identifiers
    urn:nbn:se:liu:diva-109289 (URN)10.1002/celc.201300204 (DOI)000338296100010 ()
    Available from: 2014-08-11 Created: 2014-08-11 Last updated: 2017-11-03Bibliographically approved
    6. Evaluation of the electrochemically active surface area of microelectrodes by capacitive and faradaic currents
    Open this publication in new window or tab >>Evaluation of the electrochemically active surface area of microelectrodes by capacitive and faradaic currents
    (English)Manuscript (preprint) (Other academic)
    Abstract [en]

    Two methods to estimate the electrochemically active surface area (EASA) of microelectrodes were compared. One is based on electrocapacitive measurements and the other on faradaic measuements. A systematic study revealed a strong influence of the surface roughness and the electrolyte concentration on the EASA of microelectrodes estimated from the electrocapacitive measurements, yielding a lack of reliability compared to the faradaic method.

    Keywords
    Electrochemically active surface area, microelectrode, microband, roughness, capacitive process, faradaic process
    National Category
    Chemical Sciences Chemical Engineering Chemical Process Engineering
    Identifiers
    urn:nbn:se:liu:diva-125240 (URN)
    Available from: 2016-02-17 Created: 2016-02-17 Last updated: 2017-11-03Bibliographically approved
    7. Total phenol analysis of weakly supported water using a laccase-based microband biosensor.
    Open this publication in new window or tab >>Total phenol analysis of weakly supported water using a laccase-based microband biosensor.
    Show others...
    2016 (English)In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 907, p. 45-53Article in journal (Refereed) Published
    Abstract [en]

    The monitoring of phenolic compounds in wastewaters in a simple manner is of great importance for environmental control. Here, a novel screen printed laccase-based microband array for in situ, total phenol estimation in wastewaters and for water quality monitoring without additional sample pre-treatment is presented. Numerical simulations using the finite element method were utilized for the characterization of micro-scale graphite electrodes. Anodization followed by covalent modification was used for the electrode functionalization with laccase. The functionalization efficiency and the electrochemical performance in direct and catechol-mediated oxygen reduction were studied at the microband laccase electrodes and compared with macro-scale electrode structures. The reduction of the dimensions of the enzyme biosensor, when used under optimized conditions, led to a significant improvement in its analytical characteristics. The elaborated microsensor showed fast responses towards catechol additions to tap water – a weakly supported medium – characterized by a linear range from 0.2 to 10 μM, a sensitivity of 1.35 ± 0.4 A M−1 cm−2 and a dynamic range up to 43 μM. This enhanced laccase-based microsensor was used for water quality monitoring and its performance for total phenol analysis of wastewater samples from different stages of the cleaning process was compared to a standard method.

    Place, publisher, year, edition, pages
    Elsevier, 2016
    Keywords
    Laccase; microelectrode; microband; electrochemical modeling; total phenol analysis; wastewater
    National Category
    Analytical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-123677 (URN)10.1016/j.aca.2015.12.006 (DOI)000368422900005 ()
    Note

    Funding agencies: Swedish research council Formas [245-2010-1062]; research centre Security Link [VINNOVA 2009-00966]; Norrkopings fond for Forskning och Utveckling; VINNOVA

    Available from: 2016-01-07 Created: 2016-01-07 Last updated: 2017-12-01Bibliographically approved
    8. Electrocatalytic Currents from Single Enzyme Molecules
    Open this publication in new window or tab >>Electrocatalytic Currents from Single Enzyme Molecules
    2016 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 138, no 8, p. 2504-2507Article in journal (Refereed) Published
    Abstract [en]

    Single molecule enzymology provides an opportunity to examine details of enzyme mechanisms that are not distinguishable in biomolecule ensemble studies. Here we report, for the first time, detection of the current produced in an electrocatalytic reaction by a single redox enzyme molecule when it collides with an ultramicroelectrode. The catalytic process provides amplification of the current from electron-transfer events at the catalyst leading to a measurable current. This new methodology monitors turnover of a single enzyme molecule. The methodology might complement existing single molecule techniques, giving further insights into enzymatic mechanisms and filling the gap between fundamental understanding of biocatalytic processes and their potential for bioenergy production.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2016
    National Category
    Chemical Sciences Chemical Engineering Chemical Process Engineering
    Identifiers
    urn:nbn:se:liu:diva-125241 (URN)10.1021/Jacs.5b13149 (DOI)000371453700011 ()
    Note

    Funding agencies:  Swedish research council Formas [245-2010-1062]; research center Security Link (VINNOVA ) [2009-00966]; Centre in Nano Science and Technology (CeNano, Linkoping University)

    Vid tiden för dispuation förelåg publikationen endast som manuskript

    Available from: 2016-02-17 Created: 2016-02-17 Last updated: 2017-11-30Bibliographically approved
  • 7.
    Sekretaryova, Alina
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Novel reagentless electrodes for biosensing2014Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Analytical chemical information is needed in all areas of human activity including health care, pharmacology, food control and environmental chemistry. Today one of the main challenges in analytical chemistry is the development of methods to perform accurate and sensitive rapid analysis and monitoring of analytes in ‘real’ samples. Electrochemical biosensors are ideally suited for these applications.

    Despite the wide application of electrochemical biosensors, they have some limitations. Thus, there is a demand on improvement of biosensor performance together with a necessity of simplification required for their mass production. In this thesis the work is focused on the development of electrochemical sensors with improved performance applicable for mass production, e.g. by screen printing.

    Biosensors using immobilized oxidases as the bio-recognition element are among the most widely used electrochemical devices. Electrical communication between redox enzymes and electrodes can be established by using natural or synthetic electron carriers as mediators. However, sensors based on soluble electronshuttling redox couples have low operational stability due to the leakage of water-soluble mediators to the solution. We have found a new hydrophobic mediator for oxidases – unsubstituted phenothiazine. Phenothiazine and glucose oxidase, lactate oxidase or cholesterol oxidase were successfully co-immobilized in a sol-gel membrane on a screen-printed electrode to construct glucose, lactate and cholesterol biosensors, respectively. All elaborated biosensors with phenothiazine as a mediator exhibited long-term operational stability. A kinetic study of the mediator has shown that phenothiazine is able to function as an efficient mediator in oxidase-based biosensors.

    To improve sensitivity of the biosensors and simplify their production we have developed a simple approach for production of graphite microelectrode arrays. Arrays of microband electrodes were produced by screen printing followed by scissor cutting, which enabled the realization of microband arrays at the cut edge. The analytical performance of the system is illustrated by the detection of ascorbic acid through direct oxidation and by detection of glucose using a phenothiazine mediated glucose biosensor. Both systems showed enhanced sensitivity due to improved mass transport. Moreover, the developed approach can be adapted to automated electrode recovery.

    Finally, two enzyme-based electrocatalytic systems with oxidation and reduction responses, respectively, have been combined into a fuel cell generating a current as an analytical output (a so-called self-powered biosensor). This was possible as a result of the development of the phenothiazine mediated enzyme electrodes, which enabled the  construction of a cholesterol biosensor with self-powered configuration. The biosensor generates a current when analyte (cholesterol) is added to the cell. The biosensor has been applied for whole plasma analysis.

    All developed concepts in the thesis are compatible with a wide range of applications and some of them may even be possible to realize in a fully integrated biosensor unit based on printed electronics.

    List of papers
    1. Reagentless Biosensor Based on Glucose Oxidase Wired by the Mediator Freely Diffusing in Enzyme Containing Membrane
    Open this publication in new window or tab >>Reagentless Biosensor Based on Glucose Oxidase Wired by the Mediator Freely Diffusing in Enzyme Containing Membrane
    Show others...
    2012 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 84, no 3, p. 1220-1223Article in journal (Refereed) Published
    Abstract [en]

    Wiring glucose oxidase in the membrane with an immobilized mediator is possible due to the diffusion ability of the latter, if the enzyme containing membrane is formed according to the proposed protocol, including exposing proteins to water–organic mixtures with the high content of organic solvent. In the course of the study, the new glucose oxidase mediator, unsubstituted phenothiazine, was discovered. The diffusion coefficient of the mediator in the resulting membrane is independent of the presence of enzyme. The cyclic voltammograms of the enzyme electrode after appearance of the only glucose in solution obtain a well-defined catalytic shape, which is normally observed for both the enzyme and the mediator in solution. Analytical performances of the resulting biosensor are comparable to the advanced second generation ones, which, however, require covalent linking of the mediator either to the membrane forming polymer or to the enzyme. Even without such covalent linking, the reported biosensor is characterized by an appropriate long-term operational stability allowing reagentless sensing.

    Place, publisher, year, edition, pages
    American Chemical Society (ACS), 2012
    National Category
    Analytical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-112343 (URN)10.1021/ac203056m (DOI)22206508 (PubMedID)
    Available from: 2014-11-24 Created: 2014-11-24 Last updated: 2017-12-05Bibliographically approved
    2. Unsubstituted phenothiazine as a superior water-insoluble mediator for oxidases
    Open this publication in new window or tab >>Unsubstituted phenothiazine as a superior water-insoluble mediator for oxidases
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    2014 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 53, p. 275-282Article in journal (Refereed) Published
    Abstract [en]

    The mediation of oxidases glucose oxidase (GOx), lactate oxidase (LOx) and cholesterol oxidase (ChOx) by a new electron shuttling mediator, unsubstituted phenothiazine (PTZ), was studied. Cyclic voltammetry and rotating-disk electrode measurements in nonaqueous media were used to determine the diffusion characteristics of the mediator and the kinetics of its reaction with GOx, giving a second-order rate constant of 7.6×103–2.1×104 M−1 s−1 for water–acetonitrile solutions containing 5–15% water. These values are in the range reported for commonly used azine-type mediators, indicating that PTZ is able to function as an efficient mediator. PTZ and GOx, LOx and ChOx were successfully co-immobilised in sol–gel membrane on a screen-printed electrode to construct glucose, lactate and cholesterol biosensors, respectively, which were then optimised in terms of stability and sensitivity. The electrocatalytic oxidation responses showed a dependence on substrate concentration ranging from 0.6 to 32 mM for glucose, from 19 to 565 mM for lactate and from 0.015 to 1.0 mM for cholesterol detection. Oxidation of substrates on the surface of electrodes modified with PTZ and enzyme membrane was investigated with double-step chronoamperometry and the results showed that the PTZ displays excellent electrochemical catalytic activities even when immobilised on the surface of the electrode.

    Place, publisher, year, edition, pages
    Elsevier, 2014
    Keywords
    Phenothiazine; Electron transfer mediator; Enzyme biosensor; Glucose oxidase; Lactate oxidase; Cholesterol oxidase
    National Category
    Analytical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-100391 (URN)10.1016/j.bios.2013.09.071 (DOI)000329881100044 ()
    Available from: 2013-11-05 Created: 2013-11-05 Last updated: 2017-12-06Bibliographically approved
    3. Arrays of Screen-Printed Graphite Microband Electrodes as a Versatile Electroanalysis Platform
    Open this publication in new window or tab >>Arrays of Screen-Printed Graphite Microband Electrodes as a Versatile Electroanalysis Platform
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    2014 (English)In: ChemElectroChem, ISSN 2196-0216, Vol. 1, no 4, p. 755-762Article in journal (Refereed) Published
    Abstract [en]

    Arrays of microband electrodes were developed by screen printing followed by cutting, which enabled the realization of microband arrays at the cut edge. The microband arrays of different designs were characterized by physical and electro-chemical methods. In both cases, the methods showed that the microband width was around 5 mm. Semi-steady-state cyclic voltammetry responses were observed for redox probes, and chronocoulometric measurements showed the establishment of convergent diffusion regimes characterized by current densities similar to those of a single microelectrode. The analytical performance of the electrode system and its versatility were illustrated with two electrochemical assays: detection of ascorbic acid through direct oxidation and a mediated glucose biosensor fabricated by dip coating. Due to convergent mass transport, both systems showed an enhancement in their analytical characteristics. The developed approach can be adapted to automated electrode recovery.

    Place, publisher, year, edition, pages
    Wiley, 2014
    Keywords
    graphite screen printing; microarrays; microband; sensors; voltammetry
    National Category
    Physical Sciences Chemical Sciences
    Identifiers
    urn:nbn:se:liu:diva-109289 (URN)10.1002/celc.201300204 (DOI)000338296100010 ()
    Available from: 2014-08-11 Created: 2014-08-11 Last updated: 2017-11-03Bibliographically approved
    4. Cholesterol Self-Powered Biosensor
    Open this publication in new window or tab >>Cholesterol Self-Powered Biosensor
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    2014 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 86, no 19, p. 9540-9547Article in journal (Refereed) Published
    Abstract [en]

    Monitoring the cholesterol level is of great importance, especially for people with high risk of developing heart disease. Here we report on reagentless cholesterol detection in human plasma with a novel single-enzyme, membrane-free, self-powered biosensor, in which both cathodic and anodic bioelectrocatalytic reactions are powered by the same substrate. Cholesterol oxidase was immobilized in a sol-gel matrix on both the cathode and the anode. Hydrogen peroxide, a product of the enzymatic conversion of cholesterol, was electrocatalytically reduced, by the use of Prussian blue, at the cathode. In parallel, cholesterol oxidation catalyzed by mediated cholesterol oxidase occurred at the anode. The analytical performance was assessed for both electrode systems separately. The combination of the two electrodes, formed on high surface-area carbon cloth electrodes, resulted in a self-powered biosensor with enhanced sensitivity (26.0 mA M-1 cm(-2)), compared to either of the two individual electrodes, and a dynamic range up to 4.1 mM cholesterol. Reagentless cholesterol detection with both electrochemical systems and with the self-powered biosensor was performed and the results were compared with the standard method of colorimetric cholesterol quantification.

    Place, publisher, year, edition, pages
    American Chemical Society, 2014
    National Category
    Physical Sciences Biological Sciences
    Identifiers
    urn:nbn:se:liu:diva-112176 (URN)10.1021/ac501699p (DOI)000343017100031 ()25164485 (PubMedID)
    Note

    Funding Agencies|Swedish research council Formas; research centre Security Link; Swedish Institute

    Available from: 2014-11-18 Created: 2014-11-18 Last updated: 2017-12-05
  • 8.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Karyakin, Arkady A.
    Moscow MV Lomonosov State University, Russia.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Cholesterol Self-Powered Biosensor2014In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 86, no 19, p. 9540-9547Article in journal (Refereed)
    Abstract [en]

    Monitoring the cholesterol level is of great importance, especially for people with high risk of developing heart disease. Here we report on reagentless cholesterol detection in human plasma with a novel single-enzyme, membrane-free, self-powered biosensor, in which both cathodic and anodic bioelectrocatalytic reactions are powered by the same substrate. Cholesterol oxidase was immobilized in a sol-gel matrix on both the cathode and the anode. Hydrogen peroxide, a product of the enzymatic conversion of cholesterol, was electrocatalytically reduced, by the use of Prussian blue, at the cathode. In parallel, cholesterol oxidation catalyzed by mediated cholesterol oxidase occurred at the anode. The analytical performance was assessed for both electrode systems separately. The combination of the two electrodes, formed on high surface-area carbon cloth electrodes, resulted in a self-powered biosensor with enhanced sensitivity (26.0 mA M-1 cm(-2)), compared to either of the two individual electrodes, and a dynamic range up to 4.1 mM cholesterol. Reagentless cholesterol detection with both electrochemical systems and with the self-powered biosensor was performed and the results were compared with the standard method of colorimetric cholesterol quantification.

  • 9.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Bioelectrocatalytic systems for health applications2016In: Biotechnology Advances, ISSN 0734-9750, E-ISSN 1873-1899, Vol. 34, no 3, p. 177-197Article, review/survey (Refereed)
    Abstract [en]

    We present a brief overview of bioelectrocatalytic devices for in vitro health applications, including food safety and environmental analysis, focusing on microelectrode- and microfluidic-based biosensors, paper-based point-of-care devices and wearable biosensors. The main hurdles and future perspectives are discussed. We then consider the role of electron transfer between a biocatalyst and an electrode in biosensor design. Brief descriptions of indirect, direct and mediated mechanisms are given. The principal strategies, as well as recent developments for modulation of electron transfer in biocatalytic systems are summarised. In conclusion, we highlight some of the challenges associated with improving these redox systems.

  • 10.
    Sekretaryova, Alina N.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Evaluation of the electrochemically active surface area of microelectrodes by capacitive and faradaic currentsManuscript (preprint) (Other academic)
    Abstract [en]

    Two methods to estimate the electrochemically active surface area (EASA) of microelectrodes were compared. One is based on electrocapacitive measurements and the other on faradaic measuements. A systematic study revealed a strong influence of the surface roughness and the electrolyte concentration on the EASA of microelectrodes estimated from the electrocapacitive measurements, yielding a lack of reliability compared to the faradaic method.

  • 11.
    Sekretaryova, Alina N.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony P.F.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Electrocatalytic Currents from Single Enzyme Molecules2016In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 138, no 8, p. 2504-2507Article in journal (Refereed)
    Abstract [en]

    Single molecule enzymology provides an opportunity to examine details of enzyme mechanisms that are not distinguishable in biomolecule ensemble studies. Here we report, for the first time, detection of the current produced in an electrocatalytic reaction by a single redox enzyme molecule when it collides with an ultramicroelectrode. The catalytic process provides amplification of the current from electron-transfer events at the catalyst leading to a measurable current. This new methodology monitors turnover of a single enzyme molecule. The methodology might complement existing single molecule techniques, giving further insights into enzymatic mechanisms and filling the gap between fundamental understanding of biocatalytic processes and their potential for bioenergy production.

  • 12.
    Sekretaryova, Alina N.
    et al.
    Chemistry and Material Science Faculties of M.V. Lomonosov Moscow State University, Moscow, Russia.
    Vokhmyanina, Darya V.
    Chemistry and Material Science Faculties of M.V. Lomonosov Moscow State University, Moscow, Russia.
    Chulanova, Tatyana O.
    Chemistry and Material Science Faculties of M.V. Lomonosov Moscow State University, Moscow, Russia.
    Karyakina, Elena E.
    Chemistry and Material Science Faculties of M.V. Lomonosov Moscow State University, Moscow, Russia.
    Karyakin, Arkady A.
    Chemistry and Material Science Faculties of M.V. Lomonosov Moscow State University, Moscow, Russia.
    Reagentless Biosensor Based on Glucose Oxidase Wired by the Mediator Freely Diffusing in Enzyme Containing Membrane2012In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 84, no 3, p. 1220-1223Article in journal (Refereed)
    Abstract [en]

    Wiring glucose oxidase in the membrane with an immobilized mediator is possible due to the diffusion ability of the latter, if the enzyme containing membrane is formed according to the proposed protocol, including exposing proteins to water–organic mixtures with the high content of organic solvent. In the course of the study, the new glucose oxidase mediator, unsubstituted phenothiazine, was discovered. The diffusion coefficient of the mediator in the resulting membrane is independent of the presence of enzyme. The cyclic voltammograms of the enzyme electrode after appearance of the only glucose in solution obtain a well-defined catalytic shape, which is normally observed for both the enzyme and the mediator in solution. Analytical performances of the resulting biosensor are comparable to the advanced second generation ones, which, however, require covalent linking of the mediator either to the membrane forming polymer or to the enzyme. Even without such covalent linking, the reported biosensor is characterized by an appropriate long-term operational stability allowing reagentless sensing.

  • 13.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Collision-based Electrochemistry for Investigation of Direct Electron Transfer of a Single Enzyme Molecule2017In: 26th Anniversary World Congress on Biosensors (Biosensors), Elsevier, 2017, p. 238-239Conference paper (Refereed)
    Abstract [en]

    Eldectron transfer between a biorecognition element and an electrode is an essential element of bioelectrocatalytic systems, such as biosensors and biofuel cells. The number of working systems based on direct electron communication is limited and detailed investigations of the mechanism of the process are still required. Here, we present the use of a novel approach of collision-based bioelectrocatalysis to monitor electrocatalytic currents from individual redox enzyme molecules. This approach allowed us to calculate the individual turnover rates of these molecules and investigate the influence of the applied potential, pH and additions of inhibitor on the observed rates of direct electron transfer.

  • 14.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Total phenol analysis of weakly supported water using a laccase-based microband biosensor.2016In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 907, p. 45-53Article in journal (Refereed)
    Abstract [en]

    The monitoring of phenolic compounds in wastewaters in a simple manner is of great importance for environmental control. Here, a novel screen printed laccase-based microband array for in situ, total phenol estimation in wastewaters and for water quality monitoring without additional sample pre-treatment is presented. Numerical simulations using the finite element method were utilized for the characterization of micro-scale graphite electrodes. Anodization followed by covalent modification was used for the electrode functionalization with laccase. The functionalization efficiency and the electrochemical performance in direct and catechol-mediated oxygen reduction were studied at the microband laccase electrodes and compared with macro-scale electrode structures. The reduction of the dimensions of the enzyme biosensor, when used under optimized conditions, led to a significant improvement in its analytical characteristics. The elaborated microsensor showed fast responses towards catechol additions to tap water – a weakly supported medium – characterized by a linear range from 0.2 to 10 μM, a sensitivity of 1.35 ± 0.4 A M−1 cm−2 and a dynamic range up to 43 μM. This enhanced laccase-based microsensor was used for water quality monitoring and its performance for total phenol analysis of wastewater samples from different stages of the cleaning process was compared to a standard method.

  • 15.
    Vagin, Mikhail
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology.
    Sekretareva, Alina
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Stanford Univ, CA 94305 USA; Uppsala Univ, Sweden.
    Håkansson, Anna
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphens AB, Teknikringen 1F, SE-58330 Linkoping, Sweden.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Syväjärvi, Mikael
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphens AB, Teknikringen 1F, SE-58330 Linkoping, Sweden.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphens AB, Teknikringen 1F, SE-58330 Linkoping, Sweden.
    Lundström, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Bioelectrocatalysis on Anodized Epitaxial Graphene and Conventional Graphitic Interfaces2019In: CHEMELECTROCHEM, ISSN 2196-0216, Vol. 6, no 14, p. 3791-3796Article in journal (Refereed)
    Abstract [en]

    Graphitic materials exhibit significant anisotropy due to the difference in conductivity in a single layer and between adjacent layers. This anisotropy is manifested on epitaxial graphene (EG), which can be manipulated on the nanoscale in order to provide tailor-made properties. Insertion of defects into the EG lattice was utilized here for controllable surface modification with a model biocatalyst and the properties were quantified by both electrochemical and optical methods. A comparative evaluation of the electrode reaction kinetics on the enzyme-modified 2D material vs conventional carbon electrode materials revealed a significant enhancement of mediated bioelectrocatalysis at the nanoscale.

  • 16.
    Vagin, Mikhail
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Sekretareva, Alina
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Sanchez, Rafael
    Linköping University, Department of Physics, Chemistry and Biology, Applied Physics. Linköping University, The Institute of Technology.
    Lundström, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Winquist, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Arrays of Screen-Printed Graphite Microband Electrodes as a Versatile Electroanalysis Platform2014In: ChemElectroChem, ISSN 2196-0216, Vol. 1, no 4, p. 755-762Article in journal (Refereed)
    Abstract [en]

    Arrays of microband electrodes were developed by screen printing followed by cutting, which enabled the realization of microband arrays at the cut edge. The microband arrays of different designs were characterized by physical and electro-chemical methods. In both cases, the methods showed that the microband width was around 5 mm. Semi-steady-state cyclic voltammetry responses were observed for redox probes, and chronocoulometric measurements showed the establishment of convergent diffusion regimes characterized by current densities similar to those of a single microelectrode. The analytical performance of the electrode system and its versatility were illustrated with two electrochemical assays: detection of ascorbic acid through direct oxidation and a mediated glucose biosensor fabricated by dip coating. Due to convergent mass transport, both systems showed an enhancement in their analytical characteristics. The developed approach can be adapted to automated electrode recovery.

  • 17.
    Vagin, Mikhail Yu
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Sekretareva, Alina
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Lindgren, Petter
    Håkansson, Anna
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Lundström, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Syväjärve, Mikael
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Direct bioelectrocatalysis on anodized epitaxial graphene2015In: Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society14-18 June, 2015Malmö, Sweden, Lausanne: Bioelectrochemical Society , 2015, p. 170-170Conference paper (Other academic)
    Abstract [en]

    Graphene as a nanomaterial consisting of a single layer sheets of atoms of carbon in hexagonal arrangement is making a significant impact in variety of technologies such as energy storage and chemical analysis. The significant attention paid to this thinnest nanomaterial resulted in thousands of patent applications is due to its staggering properties. Due to the planar conjugation of the sp2bonds in graphene, two-dimensional electrical conduction is highly efficient. On the contrary, the efficiency of electron exchange at the out-of-plane of the graphene sheet is small. The significant difference of the densities of electronic states at in-plane and out-of-plane of graphene sheet determines two distinct structural contributions (basal and edge plane respectively) to the behavior of all graphitic materials yielding the chemical and electrochemical anisotropy. Being the simplest building block of graphitic materials, graphene offers the possibility to study the behavior on the simplest level of structural organization. However, the major effort of the recent electrochemical studies of graphene were done using a bulk materials based on graphene flakes possessing the domination of edges of high reactivity. The planar orientation of graphene sheets with controllable exposure of basal plane is achievable via the growth by chemical vapor deposition or by epitaxial flash annealing on crystalline structures of silicon carbide. The slow growth of graphene onto crystalline support during annealing in the inert atmosphere results in a development of a high quality graphene monolayer attached to the solid insulating support. The creation of sp3-type reactive defects on the basal plane of graphite can be achieved by anodization at high anodic potentials.

    We developed the procedure for the real-time monitoring of epitaxial graphene anodization. The changes of electrochemical properties of graphene monolayer with anodization have been comparatively investigated by electrochemical methods. The estimation of specific capacitance in pure electrolyte and in conditions of Faradaic process has been carried out. Finally, the direct electrocatalysis of laccase (Trametes versicolor) has been used as an electrode reaction to probe the reactivities of anodized epitaxial graphene and conventional carbon materials.

  • 18.
    Vagin, Mikhail
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Sekretareva, Alina
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Department of Chemistry, Stanford University, Stanford, USA.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Håkansson, Anna
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Iakimov, Tihomir
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphensic AB, Teknikringen 1F, Linköping, Sweden.
    Syväjärvi, Mikael
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphensic AB, Teknikringen 1F, Linköping, Sweden.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Graphensic AB, Teknikringen 1F, Linköping, Sweden.
    Lundström, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Monitoring of epitaxial graphene anodization2017In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 238, p. 91-98Article in journal (Refereed)
    Abstract [en]

    Anodization of a graphene monolayer on silicon carbide was monitored with electrochemical impedance spectroscopy. Structural and functional changes of the material were observed by Raman spectroscopy and voltammetry. A 21 fold increase of the specific capacitance of graphene was observed during the anodization. An electrochemical kinetic study of the Fe(CN)(6)(3) (/4) redox couple showed a slow irreversible redox process at the pristine graphene, but after anodization the reaction rate increased by several orders of magnitude. On the other hand, the Ru(NH3) (3+/2+)(6) redox couple proved to be insensitive to the activation process. The results of the electron transfer kinetics correlate well with capacitance measurements. The Raman mapping results suggest that the increased specific capacitance of the anodized sample is likely due to a substantial increase of electron doping, induced by defect formation, in the monolayer upon anodization. The doping concentration increased from less than 1 x 10(13) of the pristine graphene to 4-8 x 10(13) of the anodized graphene. (C) 2017 Elsevier Ltd. All rights reserved.

1 - 18 of 18
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