| 1. |
- Abrahamsson, Tobias, 1991-
(författare)
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Synthetic Functionalities for Ion and Electron Conductive Polymers : Applications in Organic Electronics and Biological Interfaces
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- In the search for understanding and communicating with all biological systems, in humans, animals, plants, and even microorganisms, we find a common language of all communicating via electrons, ions and molecules. Since the discovery of organic electronics, the ability to bridge the gap and communicate be-tween modern technology and biology has emerged. Organic chemistry pro-vides us with tools for understanding and a material platform of polymer electronics for communication. Such insights give us not only the ability to observe fundamental phenomenon but to actively design and construct materials with chemical functionalities towards better interfaces and applications. Organic electronic materials and devices have found their way to be implemented in the field of medicine for diagnostic and therapeutic purposes, but also in water purification and to help tackle the monumental task in creating the next generation of sustainable energy production and storage. Ultimately it’s safe to say that organic electronics are not going to replace our traditional technology based on inorganic materials but rather the two fields can find a way to complement each other for various purposes and applications. Compared to conventional silicon based technology, production of carbon-based organic electronic polymer materials are extremely cheap and devices can even be made flexible and soft with great compatibility towards biology. The main focus of this thesis has been developing and synthesizing new types of organic electronic and ionic conductive polymeric materials. Rational chemical design and modifications of the materials have been utilized to introduce specific functionalities to the materials. The functionalities serving the purpose to facilitate ion and electron conductive charge transport for organic electronics and with biological interface implementation of the polymer materials. Multi-functional ionic conductive hyperbranched polyglycerol polyelectrolytes (dendrolytes) were developed comprising both ionically charged groups and cross-linkable groups. The hyperbranched polyglycerol core structure of the material possesses a hydrophilic solvating platform for both ions and maintenance of solvent molecules, while being a biocompatible structure. Coupled with the peripheral charged ionic functionalities of the polymer, the dendrolyte materials are highly ionic conductive and selective towards cationic and anionic charged atoms and large molecules when implemented as ion-exchange membranes. Homogenous ion-exchange membrane casting has been achieved by the implementation of cross-linkable functionalities in the dendrolytes, utilizing robust click-chemistry for efficient micro and macro fabrication processing of the ion-ex-change membranes for organic electronic devices. The ion-exchange membrane material was implemented in electrophoretic drug delivery devices (organic electronic ion pumps), which are used for delivery of ions and neurotransmitters with spatiotemporal resolution and are able to communicate and be used for therapeutic drug delivery purposes in biological interfaces. The dendrolyte materials were also able to form free-standing membranes, making it possible for implementation in fuel cell and desalination purposes. Trimeric conjugated thiophene pre-polymer structures were also developed in the thesis and synthesized for the purpose of implementation of the material in vivo to form electrically conductive polymer structures, and in such manner to be able to create electrodes and ultimately to connect with the central nervous system. The conjugated pre-polymers being both water soluble and enzymatically polymerizable serve as a platform to realize such a concept. Also, modifying the trimeric structure with cross-linkable functionality created the capability to form better interfaces and stability towards biological environments.
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| 2. |
- Donahue, Mary, et al.
(författare)
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Tailoring PEDOT properties for applications in bioelectronics
- 2020
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Ingår i: Materials science & engineering. R, Reports. - : Elsevier. - 0927-796X .- 1879-212X. ; 140
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Tidskriftsartikel (refereegranskat)abstract
- Resulting from its wide range of beneficial properties, the conjugated conducting polymer poly(3,4‐ethylenedioxythiophene) (PEDOT) is a promising material in a number of emerging applications. These material properties, particularly promising in the field of bioelectronics, include its well‐known high‐degree of mechanical flexibility, stability, and high conductivity. However, perhaps the most advantageous property is its ease of fabrication: namely, low‐cost and straight‐forward deposition processes. PEDOT processing is generally carried out at low temperatures with simple deposition techniques, allowing for significant customization of the material properties through, as highlighted in this review, both process parameter variation and the addition of numerous additives. Here we aim to review the role of PEDOT in addressing an assortment of mechanical and electronic requirements as a function of the conditions used to cast or polymerize the films, and the addition of additives such as surfactants and secondary dopants. Contemporary bioelectronic research examples investigating and utilizing the effects of these modifications will be highlighted.
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| 3. |
- Ajjan, Fátima, et al.
(författare)
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Enhancing Energy Storage Devices with Biomacromolecules in Hybrid Electrodes
- 2019
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Ingår i: Biotechnology Journal. - : WILEY-V C H VERLAG GMBH. - 1860-6768 .- 1860-7314. ; 14:12
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Forskningsöversikt (refereegranskat)abstract
- The development of energy storage devices with higher energy and power outputs, and long cycling stability is urgently required in the pursuit of the expanding challenges of electrical energy storage. The utilization of biologically renewable redox compounds holds a great potential in designing sustainable energy storage systems and contributes in reducing the dependence on fossil fuels for energy materials. Quinones are the principal redox centers in natural organic materials and play a key role as charge storage electrode materials because of their abundance, multiple forms and integration into the materials flow through the biosphere. Electrical energy storage devices and systems can be significantly improved by the combination of scalable quinone-based biomaterials with good electronic conductors. This review uses recent examples to show how biopolymers are providing new directions in the development of renewable biohybrid electrodes for energy storage devices.
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| 4. |
- Ajjan, Fátima, et al.
(författare)
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Innovative polyelectrolytes/poly(ionic liquid)s for energy and the environment
- 2017
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Ingår i: Polymer international. - : WILEY. - 0959-8103 .- 1097-0126. ; 66:8, s. 1119-1128
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Forskningsöversikt (refereegranskat)abstract
- This paper presents the work carried out within the European project RENAISSANCE-ITN, which was dedicated to the development of innovative polyelectrolytes for energy and environmental applications. Within the project different types of innovative polyelectrolytes were synthesized such as poly(ionic liquid)s coming from renewable or natural ions, thiazolium cations, catechol functionalities or from a new generation of cheap deep eutectic monomers. Further, macromolecular architectures such as new poly(ionic liquid) block copolymers and new (semi)conducting polymer/polyelectrolyte complexes were also developed. As the final goal, the application of these innovative polymers in energy and the environment was investigated. Important advances in energy storage technologies included the development of new carbonaceous materials, new lignin/conducting polymer biopolymer electrodes, new iongels and single-ion conducting polymer electrolytes for supercapacitors and batteries and new poly(ionic liquid) binders for batteries. On the other hand, the use of innovative polyelectrolytes in sustainable environmental technologies led to the development of new liquid and dry water, new materials for water cleaning technologies such as flocculants, oil absorbers, new recyclable organocatalyst platforms and new multifunctional polymer coatings with antifouling and antimicrobial properties. All in all this paper demonstrates the potential of poly(ionic liquid)s for high-value applications in energy and enviromental areas. (c) 2017 Society of Chemical Industry
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| 5. |
- Gabrielsson, Roger
(författare)
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Electroactive Conjugated Polyelectrolytes Based on EDOT From Synthesis to Organic Electronics
- 2012
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Conjugated polyelectrolytes (CP) show interesting electrical and optical properties for organic electronics as well as for life science applications. Their possibilities of supramolecular assembly with nanowire like misfolded proteins, amyloids, as well as synthetic polypeptides or DNA forming conducting nano composites is highly interesting as being a truly bottom up approach for fabrication of OLEDs, photovoltaic’s as well as logic devices.A special class of CPs is that of electroactive cojugated polymers (ECPs), which, due to their structure, will exhibits a unique combination of properties, including the following; electrically conducting, ability to store an electric charge and ability to exchange ions. The positive or negative excess charge can be introduced into the conjugated polymer by means of chemical or electrochemical oxidation/reduction (a process called doping) following the polymerization reaction. In order to preserve overall electroneutrality of the polymer during introduction of excess charge, ionexhange processes occurs between the polymer phase and the surrounding electrolyte solution. This charge/discharge process can be utilized for application such as; pseudo super capacitors (energy storage through oxidation/reduction processes), electro mechanical actuators (convert electrical energy to mechanical energy) and sensors (converts a chemical signal to electrical conductivity).In this thesis we describes the synthetic challenges with ECPs for applications vide supra. These mostly relates to solubility, ionic functionalization, conductivity and macromolecular properties such as size and shape of the ECPs. The key requirement in the synthesis of ECPs is that the conjugated nature of the monomer is conserved in the synthesis process and that insertion of excess charge (doping) can be obtained. This limits both the choice of monomer and the choice of polymerization process. Monomers of great complexity have been synthesized with this careful goal in mind. Furthermore, the development of novel monomers must also target the appropriate functionality for polymerization. As such, most ECP monomers are electron-rich molecules with pendant groups containing pyrroles, thiophenes, or 3,4-ethylenedioxythiophenes. These three well known ECP monomers are excellent additions to conjugated systems as they typically enable electrochemical polymerization and direct the polymerizations toward linear polymers with good stability towards doping.The first topic of this thesis we demonstrate how we can obtain water soluble ECPs with good electrical conductivity by controlling the polymerization techniques and proper ionic functionalization of the monomer. We also show how these polymers can be incorporated by self-assembly with biomolecular templates, such as, DNA and amyloid fibrils, thus generating novel electrically conductive nanowires.The second topics of this thesis demonstrate how hydrogels of ECPs can be used as bioand charge storage materials, were we demonstrate electronically controlled cell release for biology applications. Both applications are based on ECPs ability to ionexhange processes during electrochemical redox reactions. As well as ions, solvent and other neutral molecules may enter the film during charge/discharge processes. This cause a swelling or shrinking of the ECP films and the expansion and contraction of the polymer network in conjugation with the sorption/desorption of solvent molecules and ions can be described in terms of mechanical work.In the first case we were able to synthesize a water soluble ECP with high amphiphilic character. The polymer was immobilized onto a flexible electrode, suitable for cell growth and subjected to a cell growth media. When the desired cell layer was formed we applied a potential to the flexible electrode. This resulted in that the mechanical work of the immobilized ECP during the applied potential overcame the week adhesive forces to the flexible electrode, which resulted in super swelling and disintegration of the ICP and the cell layer could be harvested.In the second case the possibilities of using synthetically modified ECPs as a dopant during electropolymerization of another ECP monomer to obtain a polymer integrated network with high charge density and good charge transport properties. We demonstrate how this polymer network can be used as porous electrodes suitable for supercapacitors.
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| 6. |
- Hernández, Guiomar, et al.
(författare)
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Polyimide-polyether bindersediminishing the carbon content in lithium-sulfur batteries
- 2017
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Ingår i: Materials Today Energy. - : Elsevier BV. - 2468-6069. ; 6, s. 264-270
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Tidskriftsartikel (refereegranskat)abstract
- Lithium-sulfur batteries are on the run to become the next generation energy storage technology. First of all due to its high theoretical energy density but also for its sustainability and low cost. However, there are still several challenges to take into account such as reducing the shuttle effect, decreasing the amount of conductive carbon to increase the energy density or enhancing the sulfur utilization. Herein, redox-active binders based on polyimide-polyether copolymers have been proposed as a solution to those drawbacks. These multiblock copolymers combine the ability of poly (ethylene oxide) to act as polysulfide trap and the properties of the imide groups to redox mediate the charge-discharge of sulfur. Thus, poly (ethylene oxide) block helps with the shuttle effect and mass transport in the electrode whereas the polyimide part enhances the charge transfer promoting the sulfur utilization. Sulfur cathodes containing pyromellitic, naphthalene or perylene polyimide-polyether binders featured improved cell performance in comparison with pure PEO binder. Among them, the electrode with naphthalene polyimide-PEO binder showed the best results with an initial capacity of 1300 mA h g(-1) at C/5, low polarization and 70% capacity retention after 30 cycles. Reducing the amount of carbon black in the cathode to 5 wt%, the cell with the redox-active binder was able to deliver 500 mA h g(-1) at C/5 with 78% capacity retention after 20 cycles. Our results demonstrate the possibility to reduce the amount of carbon by introducing polyimide-polyether copolymers as redox-active binders, increasing the sulfur utilization, redox kinetics and stability of the cell. (C) 2017 Elsevier Ltd. All rights reserved.
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| 7. |
- Huang, Xiao, 1987-
(författare)
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Conducting Redox Polymers for Electrode Materials : Synthetic Strategies and Electrochemical Properties
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Organic electrode materials represent an intriguing alternative to their inorganic counterparts due to their sustainable and environmental-friendly properties. Their plastic character allows for the realization of light-weight, versatile and disposable devices for energy storage. Conducting redox polymers (CRPs) are one type of the organic electrode materials involved, which consist of a π-conjugated polymer backbone and covalently attached redox units, the so-called pendant. The polymer backbone can provide conductivity while it is oxidized or reduced (i. e., p- or n-doped) and the concurrent redox chemistry of the pendant provides charge capacity. The combination of these two components enables CRPs to provide both high charge capacity and high power capability. This dyad polymeric framework provides a solution to the two main problems associated with organic electrode materials based on small molecules: the dissolution of the active material in the electrolyte, and the sluggish charge transport within the material. This thesis introduces a general synthetic strategy to obtain the monomeric CRPs building blocks, followed by electrochemical polymerization to afford the active CRPs material. The choice of pendant and of polymer backbone depends on the potential match between these two components, i.e. the redox reaction of the pendant and the doping of backbone occurring within the same potential region. In the thesis, terephthalate and polythiophene were selected as the pendant and polymer backbone respectively, to get access to low potential CRPs. It was found that the presence of a non-conjugated linker between polymer backbone and pendant is essential for the polymerizability of the monomers as well as for the preservation of individual redox activities. The resulting CRPs exhibited fast charge transport within the polymer film and low activation barriers for charge propagation. These low potential CRPs were designed as the anode materials for energy storage applications. The combination of redox active pendant as charge carrier and a conductive polymer backbone reveals new insights into the requirements of organic matter based electrical energy storage materials.
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| 8. |
- Åkerlund, Lisa, 1986-, et al.
(författare)
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In situ Investigations of a Proton Trap Material: A PEDOT-Based Copolymer with Hydroquinone and Pyridine Side Groups Having Robust Cyclability in Organic Electrolytes and Ionic Liquids
- 2019
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 2:6, s. 4486-4495
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Tidskriftsartikel (refereegranskat)abstract
- A conducting redox polymer based on PEDOT with hydroquinone and pyridine pendant groups is reported and characterized as a proton trap material. The proton trap functionality, where protons are transferred from the hydroquinone to the pyridine sites, allows for utilization of the inherently high redox potential of the hydroquinone pendant group (3.3 V versus Li0/+) and sustains this reaction by trapping the protons within the polymer, resulting in proton cycling in an aprotic electrolyte. By disconnecting the cycling ion of the anode from the cathode, the choice of anode and electrolyte can be extensively varied and the proton trap copolymer can be used as cathode material for all-organic or metal-organic batteries. In this study, a stable and nonvolatile ionic liquid was introduced as electrolyte media, leading to enhanced cycling stability of the proton trap compared to cycling in acetonitrile, which is attributed to the decreased basicity of the solvent. Various in situ methods allowed for in-depth characterization of the polymer’s properties based on its electronic transitions (UV–vis), temperature-dependent conductivity (bipotentiostatic CV-measurements), and mass change (EQCM) during the redox cycle. Furthermore, FTIR combined with quantum chemical calculations indicate that hydrogen bonding interactions are present for all the hydroquinone and quinone states, explaining the reversible behavior of the copolymer in aprotic electrolytes, both in three-electrode setup and in battery devices. These results demonstrate the proton trap concept as an interesting strategy for high potential organic energy storage materials.
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