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Understanding the Capacitance of PEDOT:PSS
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0003-2930-676X
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2017 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 27, no 28, 1700329Article in journal (Refereed) Published
Abstract [en]

Poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) is the most studied and explored mixed ion-electron conducting polymer system. PEDOT: PSS is commonly included as an electroactive conductor in various organic devices, e.g., supercapacitors, displays, transistors, and energy-converters. In spite of its long-term use as a material for storage and transport of charges, the fundamentals of its bulk capacitance remain poorly understood. Generally, charge storage in supercapacitors is due to formation of electrical double layers or redox reactions, and it is widely accepted that PEDOT: PSS belongs to the latter category. Herein, experimental evidence and theoretical modeling results are reported that significantly depart from this commonly accepted picture. By applying a two-phase, 2D modeling approach it is demonstrated that the major contribution to the capacitance of the two-phase PEDOT: PSS originates from electrical double layers formed along the interfaces between nanoscaled PEDOT-rich and PSS-rich interconnected grains that comprises two phases of the bulk of PEDOT: PSS. This new insight paves a way for designing materials and devices, based on mixed ion-electron conductors, with improved performance.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH , 2017. Vol. 27, no 28, 1700329
Keyword [en]
cyclic voltammetry; double layers; Nernst-Planck-Poisson modeling; PEDOT:PSS; supercapacitance
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-139550DOI: 10.1002/adfm.201700329ISI: 000406183100003OAI: oai:DiVA.org:liu-139550DiVA: diva2:1130132
Note

Funding Agencies|The Swedish Energy Agency [38332-1]; Swedish Research Council [245-2010-1062]; Research Centre Security Link [VINNOVA 2009-00966]; Norrkopings fond for Forskning och Utveckling; CeNano; Knut and Alice Wallenberg Foundation; Swedish Foundation for Strategic Research (SSF); Advanced Functional Material SFO-center at Linkoping University [2009-00971]; Swedish National Infrastructure for Computing (SNIC); European Research Council (ERC) [307596, 681881]; Knut and Alice Wallenberg Foundation (Tail of the Sun); Swedish Foundation for Strategic Research [0-3D]

Available from: 2017-08-08 Created: 2017-08-08 Last updated: 2017-08-30
In thesis
1. 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)
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Available from: 2017-03-24 Created: 2017-03-17 Last updated: 2017-08-30Bibliographically approved

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The full text will be freely available from 2018-05-15 11:58
Available from 2018-05-15 11:58

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