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Quinone Pendant Group Kinetics in Poly(pyrrol-3-ylhydroquinone)
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Nanoteknologi och funktionella material. (Nanoteknologi och Funktionella Material)
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Nanoteknologi och funktionella material.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Nanoteknologi och funktionella material.ORCID-id: 0000-0002-5496-9664
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Syntetisk organisk kemi.ORCID-id: 0000-0002-9092-261X
Vise andre og tillknytning
2014 (engelsk)Inngår i: Journal of Electroanalytical Chemistry, ISSN 0022-0728, E-ISSN 1873-2569, Vol. 735, s. 95-98Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

Herein, we investigate the kinetics of the redox processes occurring in acidic aqueous electrolyte in electropolymerized poly(pyrrol-3-ylhydroquinone), which has been proposed for electrical energy storage applications. The redox conversion of the pendant groups is found to be limited by the quinone redox kinetics in thin films, rather than by the conduction through the polypyrrole backbone. Rate constants for the elementary steps involved in this 2e, 2H+ process are reported. As the films are made thicker, a gradual transition to a diffusion limited reaction is observed. The origin of the diffusion process, as well as the elementary reaction steps limiting the pendant group redox conversion is analyzed using DFT computations. The fact that the electron transport through the thin film conducting polymer backbone is not limiting the quinone reaction kinetics should allow for design of battery electrodes with high rate capabilities based on the studied material.

sted, utgiver, år, opplag, sider
2014. Vol. 735, s. 95-98
HSV kategori
Forskningsprogram
Teknisk fysik med inriktning mot nanoteknologi och funktionella material
Identifikatorer
URN: urn:nbn:se:uu:diva-230487DOI: 10.1016/j.jelechem.2014.10.013ISI: 000346214800015OAI: oai:DiVA.org:uu-230487DiVA, id: diva2:745478
Tilgjengelig fra: 2014-09-10 Laget: 2014-08-26 Sist oppdatert: 2017-12-05bibliografisk kontrollert
Inngår i avhandling
1. Conducting Redox Polymers for Electrical Energy Storage: Backbone - Substituent Interactions in Quinone Polypyrrole Model Systems
Åpne denne publikasjonen i ny fane eller vindu >>Conducting Redox Polymers for Electrical Energy Storage: Backbone - Substituent Interactions in Quinone Polypyrrole Model Systems
2014 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

Organic electrical energy storage (EES) is a growing field of research that is expected to play an important role in the future, as the need for sustainable EES increases. Conducting redox polymers (CRPs), i.e. conducting polymers with incorporated redox active moieties e.g. as pendant groups (PGs), are proposed as a promising class of compounds for this purpose. Redox cycling of the PGs can be utilized for high charge storage capacity, while the conducting polymer backbone provides fast charge transport through the material. Some of the major challenges with small-molecule systems for EES could be solved by using CRPs, e.g. capacity fading due to dissolution of the active compound, and high resistance due to slow charge transport between molecules. The latter issue is often solved by adding large amounts of conducting additives to the active material, drastically lowering the specific capacity. In this project, CRPs are shown to be able to function in battery cells without any additives, making both high capacity and high power possible. Although several CRPs have been reported in the literature, very few detailed studies have been conducted on the electrochemical processes of the two systems (i.e. the conducting polymer backbone and the redox active PGs). An important factor to consider in CRP design is the possibility for interaction between the two redox systems, which could be either beneficial or detrimental to the function as EES material. In this thesis, CRP model systems composed of hydroquinone functionalized polypyrrole have been studied, and they exhibit separate redox reactions for the PGs and the backbone, overlapping in potential. Significant interaction between them was observed, as oxidation of the PGs has severe impact on the backbone: When the oxidized and hydrophobic p-benzoquinone PGs are formed, they pack and force the polymer backbone to twist, localizing the bipolarons, and decreasing the conductivity. This is accompanied by a contraction of the polymer film and expulsion of electrolyte. Overall, the interaction in these polymers is destructive for their EES function, and it could be eliminated by introduction of a long linker unit between the PGs and the backbone.

sted, utgiver, år, opplag, sider
Uppsala: Acta Universitatis Upsaliensis, 2014. s. 72
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1177
Emneord
Organic energy storage, Hydroquinone polymers, Functionalized polypyrrole, Spectroelectrochemistry, Electrochemical quartz crystal microbalance, In situ conductivity
HSV kategori
Identifikatorer
urn:nbn:se:uu:diva-230647 (URN)978-91-554-9033-1 (ISBN)
Disputas
2014-10-30, Polhemssalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:30 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2014-10-03 Laget: 2014-08-27 Sist oppdatert: 2015-01-23bibliografisk kontrollert

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