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Bulk electronic transport impacts on electron transfer at conducting polymer electrode-electrolyte interfaces.
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
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: 0000-0001-8478-4663
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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, article id 201806087Article 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
2018. article id 201806087
Keywords [en]
conducting polymer, electron transfer, thermogalvanic cell
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-152759DOI: 10.1073/pnas.1806087115PubMedID: 30397110OAI: oai:DiVA.org:liu-152759DiVA, id: diva2:1264452
Available from: 2018-11-20 Created: 2018-11-20 Last updated: 2018-11-28
In thesis
1. Conducting Polymer Electrodes for Thermogalvanic Cells
Open this publication in new window or tab >>Conducting Polymer Electrodes for Thermogalvanic Cells
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Fossil fuels are still the dominant (ca. 80%) energy source in our society. A significant fraction is used to generate electricity with a heat engine possessing an efficiency of approximately 35%. Therefore, about 65% of fossil fuel energy is wasted in heat. Other primary heat sources include solar and geothermal energies that can heat up solid and fluids up to 150oC. The growing demand and severe environmental impact of energy systems provide an impetus for effective management and harvesting solutions dealing with waste heat. A promising way to use waste heat is to directly convert thermal energy into electrical energy by thermoelectric generators (TEGs). Solid state TEGs are electronic devices that generate electrical power due to the thermo-diffusion of electronic charge carriers in the semiconductor upon application of the thermal field. However, there is another type of thermoelectric device that has been much less investigated; this is the thermogalvanic cell (TGCs). The TGC is an electrochemical device that consists of the electrolyte solution including a reversible redox couple sandwiched between two electrodes. In our study, we focus on iron-based organometallic molecules in aqueous electrolyte. A temperature difference (Δ𝑇) between the electrodes promotes a difference in the electrode potentials [Δ𝐸(𝑇)]. Since the electrolyte contains a redox couple acting like electronic shuttle between the two electrodes, power can be generated when the two electrodes are submitted to a temperature difference. The focus of this thesis is (i) to investigate the possibility to use conducting polymer electrodes for thermogalvanic cells as an alternative to platinum and carbon-based electrodes, (ii) to investigate the role of viscosity of the electrolyte in order to consider polymer electrolytes, (iii) to understand the mechanisms limiting the electrical power output in TGCs; and (iv) to understand the fundamentals of the electron transfer taking place at the interface between the polymer electrode and the redox molecule in the electrolyte. These findings provide an essential toolbox for further improvement in conducting polymer thermoglavanic cells and various other emerging electrochemical technologies such as fuel cells, redox flow battery, dye-sensitized solar cells and industrial electrochemical synthesis.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2018. p. 93
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1971
National Category
Energy Engineering Energy Systems Other Environmental Engineering Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-152888 (URN)10.3384/diss.diva-152888 (DOI)9789176851562 (ISBN)
Public defence
2018-12-07, K3, Kåkenhus, Campus Norrköping, Norrköping, 10:00 (English)
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Available from: 2018-11-27 Created: 2018-11-27 Last updated: 2018-11-27Bibliographically approved

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Ail, UjwalaBrooke, RobertVagin, MikhailLiu, XianjieFahlman, MatsCrispin, Xavier

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