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Wijeratne, K., Ail, U., Brooke, R., Vagin, M., Liu, X., Fahlman, M. & Crispin, X. (2018). Bulk electronic transport impacts on electron transfer at conducting polymer electrode-electrolyte interfaces.. Proceedings of the National Academy of Sciences of the United States of America (7), 11899-11904
Open this publication in new window or tab >>Bulk electronic transport impacts on electron transfer at conducting polymer electrode-electrolyte interfaces.
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2018 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, no 7, p. 11899-11904Article in journal (Refereed) Epub ahead of print
Abstract [en]

Electrochemistry is an old but still flourishing field of research due to the importance of the efficiency and kinetics of electrochemical reactions in industrial processes and (bio-)electrochemical devices. The heterogeneous electron transfer from an electrode to a reactant in the solution has been well studied for metal, semiconductor, metal oxide, and carbon electrodes. For those electrode materials, there is little correlation between the electronic transport within the electrode material and the electron transfer occurring at the interface between the electrode and the solution. Here, we investigate the heterogeneous electron transfer between a conducting polymer electrode and a redox couple in an electrolyte. As a benchmark system, we use poly(3,4-ethylenedioxythiophene) (PEDOT) and the Ferro/ferricyanide redox couple in an aqueous electrolyte. We discovered a strong correlation between the electronic transport within the PEDOT electrode and the rate of electron transfer to the organometallic molecules in solution. We attribute this to a percolation-based charge transport within the polymer electrode directly involved in the electron transfer. We show the impact of this finding by optimizing an electrochemical thermogalvanic cell that transforms a heat flux into electrical power. The power generated by the cell increased by four orders of magnitude on changing the morphology and conductivity of the polymer electrode. As all conducting polymers are recognized to have percolation transport, we believe that this is a general phenomenon for this family of conductors.

Place, publisher, year, edition, pages
National academy of sciences, 2018
Keywords
conducting polymer, electron transfer, thermogalvanic cell
National Category
Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-152759 (URN)10.1073/pnas.1806087115 (DOI)000450642800036 ()30397110 (PubMedID)
Note

Funding agencies: Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University Faculty Grant [SFO-Mat-LiU 2009-00971]

Available from: 2018-11-20 Created: 2018-11-20 Last updated: 2018-12-13
Che, C., Vagin, M., Wijeratne, K., Zhao, D., Warczak, M., Jonsson, M. & Crispin, X. (2018). Conducting Polymer Electrocatalysts for Proton-Coupled Electron Transfer Reactions: Toward Organic Fuel Cells with Forest Fuels. Advanced Sustainable Systems, 317
Open this publication in new window or tab >>Conducting Polymer Electrocatalysts for Proton-Coupled Electron Transfer Reactions: Toward Organic Fuel Cells with Forest Fuels
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2018 (English)In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 317Article in journal (Refereed) Epub ahead of print
Abstract [en]

Lignin is one of the most abundant biopolymers, constituting 25% of plants. The pulp and paper industries extract lignin in their process and today seek new applications for this by-product. Here, it is reported that the aromatic alcohols obtained from lignin depolymerization can be used as fuel in high power density electrical power sources. This study shows that the conducting polymer poly(3,4-ethylenedioxythiophene), fabricated from abundant ele-ments via low temperature synthesis, enables efficient, direct, and reversible chemical-to-electrical energy conversion of aromatic alcohols such as lignin residues in aqueous media. A material operation principle related to the rela-tively high molecular diffusion and ionic conductivity within the conducting polymer matrix, ensuring efficient uptake of protons in the course of proton-coupled electron transfers between organic molecules is proposed.

Place, publisher, year, edition, pages
Wiley-Blackwell, 2018
National Category
Chemical Sciences
Identifiers
urn:nbn:se:liu:diva-148575 (URN)10.1002/adsu.201800021 (DOI)
Available from: 2018-06-13 Created: 2018-06-13 Last updated: 2018-06-26
Shtepliuk, I. I., Vagin, M., Ivanov, I. G., Iakimov, T., Yazdi, G. & Yakimova, R. (2018). Lead (Pb) interfacing with epitaxial graphene. Physical Chemistry, Chemical Physics - PCCP, 20(25), 17105-17116
Open this publication in new window or tab >>Lead (Pb) interfacing with epitaxial graphene
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 25, p. 17105-17116Article in journal (Refereed) Published
Abstract [en]

Here, we report the electrochemical deposition of lead (Pb) as a model metal on epitaxial graphene fabricated on silicon carbide (Gr/SiC). The kinetics of electrodeposition and morphological characteristics of the deposits were evaluated by complementary electrochemical, physical and computational methods. The use of Gr/SiC as an electrode allowed the tracking of lead-associated redox conversions. The analysis of current transients passed during the deposition revealed an instantaneous nucleation mechanism controlled by convergent mass transport on the nuclei locally randomly distributed on epitaxial graphene. This key observation of the deposit topology was confirmed by low values of the experimentally-estimated apparent diffusion coefficient, Raman spectroscopy and scanning electron microscopy (SEM) studies. First principles calculations showed that the nucleation of Pb clusters on the graphene surface leads to weakening of the interaction strength of the metal-graphene complex, and only spatially separated Pb adatoms adsorbed on bridge and/or edge-plane sites can affect the vibrational properties of graphene. We expect that the lead adatoms can merge in large metallic clusters only at defect sites that reinforce the metal-graphene interactions. Our findings provide valuable insights into both heavy metal ion electrochemical analysis and metal electroplating on graphene interfaces that are important for designing effective detectors of toxic heavy metals.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-149854 (URN)10.1039/c8cp01814f (DOI)000436571800024 ()29896595 (PubMedID)
Note

Funding Agencies|VR grant [621-2014-5805]; SSF [SSF GMT14-0077, SSF RMA15-0024]; Angpanneforeningens Forskningsstiftelse [16-541]

Available from: 2018-08-02 Created: 2018-08-02 Last updated: 2018-08-20
Zhybak, M., Beni, V., Vagin, M., Dempsey, E., Turner, A. & Korpan, Y. (2016). Creatinine and urea biosensors based on a novel ammonium ion-selective copper-polyaniline nano-composite. Biosensors & bioelectronics, 77, 505-511
Open this publication in new window or tab >>Creatinine and urea biosensors based on a novel ammonium ion-selective copper-polyaniline nano-composite
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2016 (English)In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 77, p. 505-511Article in journal (Refereed) Published
Abstract [en]

The use of a novel ammonium ion-specific copper-polyaniline nano-composite as transducer for hydrolase-based biosensors is proposed. In this work, a combination of creatinine deaminase and urease has been chosen as a model system to demonstrate the construction of urea and creatinine biosensors to illustrate the principle. Immobilisation of enzymes was shown to be a crucial step in the development of the biosensors; the use of glycerol and lactitol as stabilisers resulted in a significant improvement, especially in the case of the creatinine, of the operational stability of the biosensors (from few hours to at least 3 days). The developed biosensors exhibited high selectivity towards creatinine and urea. The sensitivity was found to be 85±3.4 mA M−1 cm−2 for the creatinine biosensor and 112±3.36 mA M−1 cm−2 for the urea biosensor, with apparent Michaelis–Menten constants (KM,app), obtained from the creatinine and urea calibration curves, of 0.163 mM for creatinine deaminase and 0.139 mM for urease, respectively. The biosensors responded linearly over the concentration range 1–125 µM, with a limit of detection of 0.5 µM and a response time of 15 s.

The performance of the biosensors in a real sample matrix, serum, was evaluated and a good correlation with standard spectrophotometric clinical laboratory techniques was found.

Place, publisher, year, edition, pages
Elsevier, 2016
Keywords
Creatinine; Urea; Amperometric ammonium detection; Copper polyanilinecomposite
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:liu:diva-123681 (URN)10.1016/j.bios.2015.10.009 (DOI)000366766900073 ()26457736 (PubMedID)
Projects
SMARTCABCERSENS
Funder
EU, FP7, Seventh Framework Programme, PIRSES-GA-2012-318053
Note

Funding agencies: SMARTCANCERSENS

Available from: 2016-01-08 Created: 2016-01-08 Last updated: 2017-12-01Bibliographically approved
Zhybak, M. T., Vagin, M. Y., Beni, V., Liu, X., Dempsey, E., Turner, A. P. F. & Korpan, Y. I. (2016). Direct detection of ammonium ion by means of oxygen electrocatalysis at a copper-polyaniline composite on a screen-printed electrode.. Microchimica Acta, 183(6), 1981-1987
Open this publication in new window or tab >>Direct detection of ammonium ion by means of oxygen electrocatalysis at a copper-polyaniline composite on a screen-printed electrode.
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2016 (English)In: Microchimica Acta, ISSN 0026-3672, E-ISSN 1436-5073, Vol. 183, no 6, p. 1981-1987Article in journal (Refereed) Published
Abstract [en]

A novel electrocatalytic material for oxygen reduction, based on polyaniline in combinationwith copper, was developed and utilised for the direct voltammetric quantification of ammonium ions. Consecutive electrode modification by electrodeposited copper, a Nafion membrane and electropolymerised polyaniline resulted in an electrocatalytic composite material which the retained conductivity at neutral pH. Ammonia complex formation with Cu (I) caused the appearance of oxygen electrocatalysis, which was observed as an increase in cathodic current. This Faradaic phenomenon offered the advantage of direct voltammetric detection and was utilised for ammonium electroanalysis. The developed quantification protocol was applied for ammonium assay in human serum and compared with the routine approach for clinical analysis.

Keywords
Conductive polymer, Nanocomposite, Amperometry, Electrochemical impedance spectroscopy, SEM, EDX, XPS, Serum analysis
National Category
Other Basic Medicine
Identifiers
urn:nbn:se:liu:diva-128192 (URN)10.1007/s00604-016-1834-3 (DOI)000376600300021 ()
Funder
EU, FP7, Seventh Framework Programme, PIRSES
Available from: 2016-05-20 Created: 2016-05-20 Last updated: 2018-03-23
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)

Vid tiden för dispuation förelåg publikationen endast som manuskript

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
Zeglio, E., Vagin, M., Musumeci, C., Ajjan, F., Gabrielsson, R., Trinh, X. t., . . . Inganäs, O. (2015). Conjugated Polyelectrolyte Blends for Electrochromic and Electrochemical Transistor Devices. Chemistry of Materials, 27(18), 6385-6393
Open this publication in new window or tab >>Conjugated Polyelectrolyte Blends for Electrochromic and Electrochemical Transistor Devices
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2015 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 27, no 18, p. 6385-6393Article in journal (Refereed) Published
Abstract [en]

Two self-doped conjugated polyelectrolytes, having semiconducting and metallic behaviors, respectively, have been blended from aqueous solutions in order to produce materials with enhanced optical and electrical properties. The intimate blend of two anionic conjugated polyelectrolytes combine the electrical and optical properties of these, and can be tuned by blend stoichiometry. In situ conductance measurements have been done during doping of the blends, while UV vis and EPR spectroelectrochemistry allowed the study of the nature of the involved redox species. We have constructed an accumulation/depletion mode organic electrochemical transistor whose characteristics can be tuned by balancing the stoichiometry of the active material.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2015
National Category
Materials Chemistry Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-122212 (URN)10.1021/acs.chemmater.5b02501 (DOI)000361935000028 ()
Note

Funding Agencies|Marie Curie network "Renaissance"; Knut and Alice Wallenberg foundation through Wallenberg Scholar grant; Swedish Research Council [VR-2014-3079, D0556101]; Carl Trygger Foundation [CTS 12:206]

Available from: 2015-10-26 Created: 2015-10-23 Last updated: 2017-12-01
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
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-8478-4663

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