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Total phenol analysis of weakly supported water using a laccase-based microband biosensor.
Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. (Laboratory of Organic Electronics)
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. (Laboratory of Organic Electronics)
Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-1815-9699
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2016 (English)In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 907, 45-53 p.Article 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. Vol. 907, 45-53 p.
Keyword [en]
Laccase; microelectrode; microband; electrochemical modeling; total phenol analysis; wastewater
National Category
Analytical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-123677DOI: 10.1016/j.aca.2015.12.006ISI: 000368422900005OAI: oai:DiVA.org:liu-123677DiVA: diva2:891808
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: 2017-03-17Bibliographically approved
In thesis
1. Facilitating electron transfer in bioelectrocatalytic systems
Open this publication in new window or tab >>Facilitating electron transfer in bioelectrocatalytic systems
2016 (English)Doctoral 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.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2016. 74 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1738
National Category
Chemical Sciences Chemical Engineering Chemical Process Engineering
Identifiers
urn:nbn:se:liu:diva-125242 (URN)10.3384/diss.diva-125242 (DOI)978-91-7685-841-7 (ISBN)
Public defence
2016-03-18, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2016-02-17 Created: 2016-02-17 Last updated: 2016-03-08Bibliographically approved
2. Ionic and electronic transport in electrochemical and polymer based systems
Open this publication in new window or tab >>Ionic and electronic transport in electrochemical and polymer based systems
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Electrochemical systems, which rely on coupled phenomena of the chemical change and electricity, have been utilized for development an interface between biological systems and conventional electronics.  The development and detailed understanding of the operation mechanism of such interfaces have a great importance to many fields within life science and conventional electronics. Conducting polymer materials are extensively used as a building block in various applications due to their ability to transduce chemical signal to electrical one and vice versa. The mechanism of the coupling between the mass and charge transfer in electrochemical systems, and particularly in conductive polymer based system, is highly complex and depends on various physical and chemical properties of the materials composing the system of interest.

The aims of this thesis have been to study electrochemical systems including conductive polymer based systems and provide knowledge for future development of the devices, which can operate with both chemical and electrical signals. Within the thesis, we studied the operation mechanism of ion bipolar junction transistor (IBJT), which have been previously utilized to modulate delivery of charged molecules. We analysed the different operation modes of IBJT and transition between them on the basis of detailed concentration and potential profiles provided by the model.

We also performed investigation of capacitive charging in conductive PEDOT:PSS polymer electrode. We demonstrated that capacitive charging of PEDOT:PSS electrode at the cyclic voltammetry, can be understood within a modified Nernst-Planck-Poisson formalism for two phase system in terms of the coupled ion-electron diffusion and migration without invoking the assumption of any redox reactions.

Further, we studied electronic structure and optical properties of a self-doped p-type conducting polymer, which can polymerize itself along the stem of the plants. We performed ab initio calculations for this system in undoped, polaron and bipolaron electronic states. Comparison with experimental data confirmed the formation of undoped or bipolaron states in polymer film depending on applied biases.

Finally, we performed simulation of the reduction-oxidation reaction at microband array electrodes. We showed that faradaic current density at microband array electrodes increases due to non-linear mass transport on the microscale compared to the corresponding macroscale systems.  The studied microband array electrode was used for developing a laccase-based microband biosensor. The biosensor revealed improved analytical performance, and was utilized for in situ phenol detection.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2017. 49 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1841
Keyword
Modeling, Charge transport, Charge carriers Electrochemical systems, Polymer, PEDOT:PSS, Supercapacitance, Cyclic voltammetry, double layers, Nernst-Planck-Poisson, DFT, TDDFT, Ion Bipolar Junction Transistor, ETE-S
National Category
Materials Chemistry Condensed Matter Physics Inorganic Chemistry Textile, Rubber and Polymeric Materials
Identifiers
urn:nbn:se:liu:diva-135429 (URN)10.3384/diss.diva-1082793 (DOI)9789176855485 (ISBN)
Public defence
2017-04-25, K3, Kåkenhus, Campus Norrköping, Norrköping, 10:15 (English)
Opponent
Supervisors
Available from: 2017-03-24 Created: 2017-03-17 Last updated: 2017-08-30Bibliographically approved

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