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Sekretaryova, A., Eriksson, M. & Turner, A. (2016). Bioelectrocatalytic systems for health applications. Biotechnology Advances, 34(3), 177-197
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
Sekretaryova, A. N., Vagin, M. Y., Turner, A. P. .. & Eriksson, M. (2016). Electrocatalytic Currents from Single Enzyme Molecules. Journal of the American Chemical Society, 138(8), 2504-2507
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)

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Available from: 2016-02-17 Created: 2016-02-17 Last updated: 2017-11-30Bibliographically approved
Sekretaryova, A., Volkov, A. V., Zozoulenko, I. V., Turner, A., Vagin, M. Y. & Eriksson, M. (2016). Total phenol analysis of weakly supported water using a laccase-based microband biosensor.. Analytica Chimica Acta, 907, 45-53
Open this publication in new window or tab >>Total phenol analysis of weakly supported water using a laccase-based microband biosensor.
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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
Vagin, M. Y., Jeerapan, I., Wannapob, R., Thavarungkul, P., Kanatharana, P., Anwar, N., . . . Wing Cheung, M. (2016). Water-processable polypyrrole microparticle modules for direct fabrication of hierarchical structured electrochemical interfaces. Electrochimica Acta, 190, 495-503
Open this publication in new window or tab >>Water-processable polypyrrole microparticle modules for direct fabrication of hierarchical structured electrochemical interfaces
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2016 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 190, p. 495-503Article in journal (Refereed) Published
Abstract [en]

Hierarchically structured materials (HSMs) are becoming increasingly important in catalysis, separation and energy applications due to their advantageous diffusion and flux properties. Here, we introduce a facile modular approach to fabricate HSMs with tailored functional conducting polypyrrole microparticles (PPyMP). The PPyMPs were fabricated with a calcium carbonate (CaCO3) template-assisted polymerization technique in aqueous media at room temperature, thus providing a new green chemistry for producing water-processable functional polymers. The sacrificial CaCO3 template guided the polymerization process to yield homogenous PPyMPs with a narrow size distribution. The porous nature of the CaCO3 further allows the incorporation of various organic and inorganic dopants such as an electrocatalyst and redox mediator for the fabrication of functional PPyMPs. Dawson-type polyoxometalate (POM) and methylene blue (MB) were chosen as the model electrocatalyst and electron mediator dopant, respectively. Hierarchically structured electrochemical interfaces were created simply by self-assembly of the functional PPyMPs. We demonstrate the versatility of this technique by creating two different hierarchical structured electrochemical interfaces: POM-PPyMPs for hydrogen peroxide electrocatalysis and MB-PPyMPs for mediated bioelectrocatalysis. We envision that the presented design concept could be extended to different conducting polymers doped with other functional organic and inorganic dopants to develop advanced electrochemical interfaces and to create high surface area electrodes for energy storage.

Place, publisher, year, edition, pages
Elsevier, 2016
Keywords
Polypyrrole;microparticles;hierarchical interfaces;polyoxometalate;redox mediator;electrocatalysis;bioelectrocatalysis
National Category
Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-123659 (URN)10.1016/j.electacta.2015.12.183 (DOI)000371141500060 ()
Note

Funding agencies: Development and Promotion of Science and Technology Talents projects (DPST) - Royal Thai Government; Graduate School, Prince of Songkla University, Hat Yai, Thailand

Available from: 2016-01-05 Created: 2016-01-05 Last updated: 2018-10-04
Cavanillas, S., Winquist, F. & Eriksson, M. (2015). A self-polishing platinum ring voltammetric sensor and its application to complex media. Analytica Chimica Acta, 859, 29-36
Open this publication in new window or tab >>A self-polishing platinum ring voltammetric sensor and its application to complex media
2015 (English)In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 859, p. 29-36Article in journal (Refereed) Published
Abstract [en]

A self-polishing voltammetric sensor was recently developed and has been applied to samples of urea, milk and sewage water. The polishing device continuously grinds a platinum ring electrode, offering a reproducible and clean electrode surface. Principal component analysis (PCA) and partial least squares (PLS) techniques were applied to interpret the data and to build prediction models. In an evaluation of samples with different urea concentrations, the grinding step allows for repeatable measurements, similar to those after electrochemical cleaning. Furthermore, for the determination of sewage water concentrations in drinking water and for the evaluation of different fat contents in milk samples, the polishing eliminates sensor drift produced by electrode fouling. The results show that the application of a self-polishing unit offers a promising tool for electrochemical studies of difficult analytes and complex media. (C) 2014 Elsevier B.V. All rights reserved.

Place, publisher, year, edition, pages
Elsevier Masson, 2015
Keywords
Voltammetric sensor; Electronic tongue; Urea; Milk; Drinking water; Sewage water
National Category
Biological Sciences Physical Sciences
Identifiers
urn:nbn:se:liu:diva-114563 (URN)10.1016/j.aca.2014.11.039 (DOI)000348457300003 ()25622603 (PubMedID)
Note

Funding Agencies|MICINN [BES-2010-032352]

Available from: 2015-03-02 Created: 2015-02-26 Last updated: 2017-12-04
Vagin, M. Y., Sekretareva, A., Lindgren, P., Håkansson, A., Eriksson, M., Lundström, I., . . . Yakimova, R. (2015). Direct bioelectrocatalysis on anodized epitaxial graphene. In: Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society14-18 June, 2015Malmö, Sweden: . Paper presented at Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society 14-18 June, 2015 Malmö, Sweden (pp. 170-170). Lausanne: Bioelectrochemical Society
Open this publication in new window or tab >>Direct bioelectrocatalysis on anodized epitaxial graphene
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2015 (English)In: 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, Published 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.

Place, publisher, year, edition, pages
Lausanne: Bioelectrochemical Society, 2015
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-122686 (URN)
Conference
Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society 14-18 June, 2015 Malmö, Sweden
Available from: 2015-11-16 Created: 2015-11-16 Last updated: 2017-11-03Bibliographically approved
Sekretareva, A., Vagin, M., Volkov, A. V., Zozoulenko, I. V., Turner, A. & Eriksson, M. (2015). Screen printed microband array based biosensor for water monitoring. In: The Frumkin Symposium: . Paper presented at The Frumkin Symposium, 21-23 October 2015, Moscow, Russia.
Open this publication in new window or tab >>Screen printed microband array based biosensor for water monitoring
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2015 (English)In: The Frumkin Symposium, 2015Conference paper, Oral presentation with published abstract (Refereed)
National Category
Biological Sciences
Identifiers
urn:nbn:se:liu:diva-123698 (URN)
Conference
The Frumkin Symposium, 21-23 October 2015, Moscow, Russia
Available from: 2016-01-08 Created: 2016-01-08 Last updated: 2017-11-03
Sekretareva, A., Vagin, M. Y., Volkov, A. V., Zozoulenko, I. V., Turner, A. P. .. & Eriksson, M. (2015). Total phenol analysis of water using a laccase-based microsensor array. In: Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society. 14-18 June, 2015. Malmö, Sweden: . Paper presented at The XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society. 14-18 June, 2015. Malmö, Sweden (pp. 155-155). Lausanne: Bioelectrochemical Society
Open this publication in new window or tab >>Total phenol analysis of water using a laccase-based microsensor array
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2015 (English)In: 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, Published 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.

Place, publisher, year, edition, pages
Lausanne: Bioelectrochemical Society, 2015
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:liu:diva-122687 (URN)
Conference
The XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society. 14-18 June, 2015. Malmö, Sweden
Available from: 2015-11-16 Created: 2015-11-16 Last updated: 2017-11-03Bibliographically approved
Sekretaryova, A., Beni, V., Eriksson, M., Turner, A. & Vagin, M. Y. (2014). A highly sensitive and self-powered cholesterol biosensor. In: 24th Anniversary World Congress on Biosensors – Biosensors 2014: . Paper presented at 24thAnniversary World Congress on Biosensors – Bios ensors 2014, 27-30 May 2014, Melbourne, Australia. Elsevier
Open this publication in new window or tab >>A highly sensitive and self-powered cholesterol biosensor
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2014 (English)In: 24th Anniversary World Congress on Biosensors – Biosensors 2014, Elsevier, 2014Conference paper, Oral presentation with published abstract (Other academic)
Abstract [en]

Blood cholesterol is a very important parameter for the assessment of atherosclerosis and other lipid disorders. The total cholesterol concentration in human blood should be less than 5.17 mM. Concentrations in the range 5.17 – 6.18 mM are considered borderline high risk and levels above 6.21 mM, high risk. Cholesterol determination with high accuracy is therefore necessary in order to differentiate these levels for medical screening or diagnosis. Several attempts to develop highly sensitive cholesterol biosensors have been described, but, to the best of our knowledge, this is the first report of a self-powered cholesterol biosensor, i.e. a device delivering the analytical information from the current output of the energy of the biocatalytic conversion of cholesterol, without any external power source. This is particularly relevant to the development of inexpensive screening devices based on printed electronics.

 

We present two complementary bioelectrocatalytic platforms suitable for the fabrication of a self-powered biosensor. Both are based on cholesterol oxidase (ChOx) immobilisation in a sol-gel matrix, as illustrated in Fig. 1 [1]. Mediated biocatalytic cholesterol oxidation [2] was used as the anodic reaction and electrocatalytic reduction of hydrogen peroxide on Prussian Blue (PB) as the cathodic reaction. Due to a synergistic effect in the self-powered cholesterol biosensor, the analytical parameters of the overall device exceeded those of the individual component half-cells, yielding a sensitivity of 0.19 A M-1 cm-2 and a dynamic range that embraces the free cholesterol concentrations found in human blood.

 

Thus, we have demonstrated the novel concept of highly sensitive cholesterol determination using the first self-powered cholesterol biosensor. This configuration is particularly promising for incorporation in emerging plastic- and paper-based analytical instruments for decentralised diagnostics and mobile health.

 

Place, publisher, year, edition, pages
Elsevier, 2014
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-108436 (URN)
Conference
24thAnniversary World Congress on Biosensors – Bios ensors 2014, 27-30 May 2014, Melbourne, Australia
Available from: 2014-06-27 Created: 2014-06-27 Last updated: 2017-11-03
Sekretaryova, A. N., Vagin, M. Y., Turner, A. & Eriksson, M. (2014). A screen-printed microband array biosensor for water monitoring. In: 15th International Conference on Electroanalysis (ESEAC): . Paper presented at 15th International Conference on Electroanalysis (ESEAC), 11-15 June 2014, Malmö, Sweden.
Open this publication in new window or tab >>A screen-printed microband array biosensor for water monitoring
2014 (English)In: 15th International Conference on Electroanalysis (ESEAC), 2014Conference paper, Oral presentation with published abstract (Other academic)
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-108438 (URN)
Conference
15th International Conference on Electroanalysis (ESEAC), 11-15 June 2014, Malmö, Sweden
Available from: 2014-06-27 Created: 2014-06-27 Last updated: 2017-11-03
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-0873-2877

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