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Spectroelectrochemical investigation of redox states in a polypyrrole/lignin composite electrode material
Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0003-3899-4891
Poznan University of Tech, Poland.
Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-1639-5735
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2015 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 24, p. 12927-12937Article in journal (Refereed) Published
Abstract [en]

We report spectroelectrochemical studies to investigate the charge storage mechanism of composite polypyrrole/lignin electrodes. Renewable bioorganic electrode materials were produced by electropolymerization of pyrrole in the presence of a water-soluble lignin derivative acting as a dopant. The resulting composite exhibited enhanced charge storage abilities due to a lignin-based faradaic process, which was expressed after repeated electrochemical redox of the material. The in situ FTIR spectroelectrochemistry results show the formation of quinone groups, and reversible oxidation-reduction of these groups during charge-discharge experiments in the electrode materials. The most significant IR bands include carbonyl absorption near 1705 cm(-1), which is attributed to the creation of quinone moieties during oxidation, and absorption at 1045 cm(-1) which is due to hydroquinone moieties.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2015. Vol. 3, no 24, p. 12927-12937
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-120069DOI: 10.1039/c5ta00788gISI: 000356022800044OAI: oai:DiVA.org:liu-120069DiVA, id: diva2:839931
Note

Funding Agencies|Knut and Alice Wallenberg foundation; Marie Curie network Renaissance; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]

Available from: 2015-07-06 Created: 2015-07-06 Last updated: 2017-12-04
In thesis
1. Biohybrid Polymer Electrodes for Renewable Energy Storage
Open this publication in new window or tab >>Biohybrid Polymer Electrodes for Renewable Energy Storage
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Daily and seasonally fluctuating energy supply and demand requires adequate energy storage solutions. In recent years electrochemical supercapacitors have attracted considerable attention due to their ability to both store and deliver electrical energy efficiently. Our efforts are focused on developing and optimizing sustainable organic electrode materials for supercapacitors based on renewable bioorganic materials, offering a cheap, environmentally friendly and scalable alternative to store energy. In particular, we are using the second most abundant biopolymer in nature, lignin (Lig), which is an insulating material. However, when used in combination with electroactive and conducting polymers such as polypyrrole (PPy) and poly(3,4-ethylenedioxythiophene) (PEDOT), the biohybrid electrodes PPy/Lig and PEDOT/Lig display significantly enhanced energy storage performance as compared to the pristine conducting polymers without the lignin. Redox cyclic voltammetry and galvanostatic charge/discharge measurements indicate that the enhanced performance is due to the additional pseudocapacitance generated by the quinone moieties in lignin. Moreover, a conjugated redoxpolymer poly(aminoanthraquinone) PAAQ, with intrinsic quinone functions and excellentstability, has been combined with lignin and PEDOT resulting in a trihybrid bioelectrode. PEDOT compensates the low conductivity of PAAQ and provides electrical pathways to the quinone groups. The electrochemically generated quinones undergo a two electron, two protonredox process within the biohybrid electrodes as revealed by FTIR spectroelectrochemistry.These remarkable features reveal the exciting potential of a full organic energy storage device with long cycle life. Therefore, supercapacitor devices were designed in symmetric or asymmetric two electrode configuration. The best electrochemical performance was achieved by the asymmetric supercapacitor based on PEDOT+Lignin/PAAQ as the positive electrode and PEDOT/PAAQ as the negative electrode. This device exhibits superior electrochemical performance and outstanding stability after 10000 charge/discharge cycles due to the synergistic effect of the two electrodes. Finally, we have characterized the response of this supercapacitor device when charged with the intermittent power supply from an organic photovoltaic module. We have designed charging/discharging conditions such that reserve power was available in the storage device at all times. This work has resulted in an inexpensive fully organic system witht he dual function of energy conversion and storage.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2017. p. 64
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1834
National Category
Energy Systems Renewable Bioenergy Research Energy Engineering Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-136156 (URN)9789176855737 (ISBN)
Public defence
2017-04-27, Plank, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2017-03-31 Created: 2017-03-31 Last updated: 2018-01-13Bibliographically approved
2. Application of Vibrational Spectroscopy in Organic Electronics
Open this publication in new window or tab >>Application of Vibrational Spectroscopy in Organic Electronics
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The rapid technological developments enforce us to live in an increasingly electronic world, and the revolutionary usage of conjugated polymers in electronics in the late 1970s accelerated these developments, based on the unique characteristics of conjugated polymers, such as low cost, easy processing, mechanical flexibility, large-area application and compatibility with a variety of substrates. Organic electronic devices are commercially available in the form of, for example, solar cells, transistors, and organic light-emitting diode (OLED) displays. Scientists work on electroactive polymers to enhance their chemical, electrical and mechanical properties, to improve parameters such as charge carrier mobility and doping capacity, in order to reach acceptable efficiency and stability to fabricate organic electronic devices. A comprehensive understanding of the changes in chemical structure, in response to external factors such as applied potential and temperature gradients, which can disturb the chemical equilibrium of the constituent materials, and of the conduction mechanisms of the operating devices, can help to enhance the performance of organic electronics devices. Vibrational spectroscopy is a powerful analytical method for in-situ monitoring of such chemical or electrochemical reactions and associated structural changes of conjugated polymers in a working device.

In this thesis, Fourier-transform infrared (FTIR) spectroscopy has been used to study the structural changes in electroactive organic materials, in response to chemical or electrochemical reactions, and to study electrical and thermal conduction mechanisms in different organic electronic devices. FTIR microscopy was used to approach a realistic conduction mechanism by time-resolved chemical imaging of active materials in planar light-emitting electrochemical cells (LECs), investigated as an alternative to organic light emitting diodes (OLEDs). These chemical images are used for in-situ mapping of anion density profiles, polymer doping, and dynamic junction formation in the active layer under an applied bias. Results confirm the electrochemical doping model and help the systematic improvement of function and manufacture of LECs. Mixed ion-electron polymeric conductor materials such as PEDOT-PSS are used as active materials in organic thermoelectric generators (OTEGs), where charge carrier transport through the active layer promotes internal electrochemical reactions under a temperature gradient. FTIR microscopy and FTIR-attenuated total reflection (FTIR-ATR) were used to study thermoelectric and electrical properties of the conducting polymers. Recently, electrochemical supercapacitors have emerged as an alternative to conventional batteries, and polymeric materials are used to design polymer electrodes for renewable energy storage. To understand the charge transfer and structural changes of the polymer during the redox reaction, we have used FTIR-ATR as a tool for the in-situ spectroelectrochemical study of redox states in polypyrrole/lignin composites; we clarified the structural changes in the materials during charging and discharging of the composite. In further work, FTIR-ATR was also used for in-situ spectroelectrochemical studies of PEDOT:Cl, to monitor the effects of dissolved oxygen on PEDOT:Cl films, which are used as electrodes in renewable energy technologies. Further, time-resolved oxygen reduction reactions of PEDOT:Cl have been studied via polarization-modulation infrared reflection-absorption spectroscopy (PM-IRAS) to reveal chemical changes in electrochemically doped PEDOT upon exposure to oxygen.

Taken together, these studies provide an advancement in the use of infrared spectroscopy as a tool to understand electroactive materials under wet conditions, and have provided detailed chemical and electrochemical information of materials and devices under operation, that is not easily accessible with other methods.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2017. p. 61
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1884
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:liu:diva-142216 (URN)9789176854440 (ISBN)
Public defence
2017-11-17, Planck, F-House, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2017-10-23 Created: 2017-10-23 Last updated: 2017-10-23Bibliographically approved

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Ajjan, FátimaJavad Jafari, MohammadEderth, ThomasInganäs, Olle

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