| 1. |
- Ekspong, Joakim, 1987-
(författare)
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Electrocatalysts for sustainable hydrogen energy : disordered and heterogeneous nanomaterials
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- With the current global greenhouse gas emissions, our remaining carbon budget is depleted in only 7 years. After that, several biophysical systems are predicted to collapse such as the arctic ice, coral reefs and the permafrost, leading to potentially irreversible consequences. Our emissions are strongly correlated to access of energy and even if we are aware of the planetary emergency today, our emissions still continue to grow. Electrical vehicles have the possibility to reduce the emissions in the transportation sector significantly. However, these vehicles are still expensive and impractical for long-distance or heavy transportation. While political actions and technological development are essential to keep prices down, the driving dis- tance can be increased by replacing the batteries for onboard electricity production. In hydrogen fuel cells, electricity is produced by combining hydrogen gas (H2) and oxygen with only water as the by-product and if employed in electrical vehicles, distances of 500 km are enabled with a refueling time in 5 minutes. For other uses than in vehicles, H2 is also promising for large-scale electricity storage and for several industrial processes such as manufacturing CO2-free steel, ammonia and synthetic fuels. However, today most H2 production methods relies on fossil fuels and releases huge amounts of CO2. Electrolysis of water is an alternative production method where H2, along with oxygen are produced from water. To split the water, electricity has to be added and if renewable energy sources are used, the method has zero emissions and is considered most promising for a sustainable hydrogen energy economy. The tech- nique is relatively expensive compared to the fossil fuel-based methods and relies on rare noble metals such as platinum as catalysts for decreasing the required energy to split water. For large scale productions, these metals need to be replaced by more sustainable and abundant catalysts to lower the cost and minimize the environmental impacts. In this thesis we have investigated such candidates for the water splitting reaction but also to some extent for the oxygen reduction reaction in fuel cells. By combining theory and experiments we hope to aid in the development and facilitate a transition to clean hydrogen energy. We find among other things that i) defects in catalytic materials plays a significant role the performance and efficiency, and that ii) heterogeneity influence the adsorption energies of reaction intermediates and hence the catalytic efficiency and iii) while defects are not often studied for electrocatalytic reactions, these may inspire for novel materials in the future.
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| 2. |
- Enevold, Jenny, 1981-
(författare)
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Structure and morphology control of organic semiconductors for functional optoelectronic applications
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The functionality and application of organic semiconductors are largely dependent on their constituent structure and morphology. This thesis presents a number of functional and novel approaches for the control and tuning of structural and morphological features of a variety of organic semiconductor materials, and also demonstrates that these approaches can be utilized for improved device operation of field-effect transistors, organic solar cells and light-emitting electrochemical cells.The fullerene family is a particular group of closed-cage organic semiconductors, which can be photochemically coupled into larger dimeric or polymeric structures through the excitation of the fullerene molecules by light emission. In Paper I, we perform a detailed experimental and analytical investigation, which demonstrates that this photochemical monomer-to-dimer transformation requires that both constituent fullerene molecules are photoexcited. The direct consequence is that the initial probability for the photochemical transformation is dependent on the square of the light-emission intensity.The photochemical coupling of fullerene molecules commonly results in a distinctly lowered solubility in common hydrophobic solvents, which can be utilized for the direct patterning of fullerene films by resist-free lithography. In Paper II, we utilize this patterning opportunity for the fabrication of one-dimensional fullerene nano-stripes using two-beam laser interference lithography. A desired high contrast between the patterned and non-patterned fullerene regions is facilitated by the non-linear response of the photochemical transformation process, as predicted by the findings in Paper I. The patterned fullerene nano-stripes were utilized as the active material in field-effect transistors, which featured high electron mobility and large on-off ratio.This patterning was in Paper III extended into easy tunable two-dimensional fullerene structures by the design and development of an exposure setup, essentially comprising a laser and a spatial light modulator featuring >8 millions of independently controlled mirrors. With this approach, we could fabricate well-defined fullerene microdots over a several square-millimeter sized area, which was utilized as an internal out-coupling layer in a light-emitting electrochemical cell with significantly enhanced light output.Paper IV reports on the development of a new “spray-sintering” method for the cost-efficient solution-based deposition of the active material in light-emitting electrochemical cells. This carefully designed approach effectively resolves the issue with phase separation between the hydrophobic organic semiconductor and the hydrophilic electrolyte that results in a sub-par LEC performance, and also allows for the direct fabrication of LEC devices onto complex surfaces, including a stainless-steel fork.Paper V finally reports on the design and synthesis of a soluble small molecule, featuring a donor-acceptor-donor configuration. It acts as the donor when combined with a soluble fullerene acceptor in the active material of organic solar cells, and such devices with optimized donor/acceptor nanomorphology feature a high open-circuit voltage of ~1.0 V during solar illumination.
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| 3. |
- Lindh, E. Mattias, 1986-
(författare)
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On the operation of light-emitting electrochemical cells
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- We are in the midst of a technological revolution that permeates nearly all human activities; artificial light is one of the most visible contributors in this societal change. If more efficient, green, and versatile light sources can be developed, they might improve the life of millions of people around the world while causing minimal damage to our climate and environment. The unique operational mechanism of the light-emitting electrochemical cell (LEC) makes it an ideal fit for some unconventional and emerging uses of light, in for example medicine and security.By exploiting this operational mechanism, in which mobile ions enable electrochemical doping of a luminescent polymer, we have designed and fabricated new bilayer LEC architectures. The bilayer LEC features patterned light emission that is easily adjustable during fabrication, and that can be configured to suit new applications of light. Given the light-emitting nature of the LEC, it is somewhat surprising that the optical understanding of its operation is rather limited. To fill this knowledge gap, we investigate how the optical properties of the luminescent polymer respond to electrochemical doping. We find that the complex-refractive index spectrum in the active layer of an LEC, as a direct result of the doping, varies in both space and time. The thin-film structure of an LEC implies that computational predictions of its luminous output need to consider internal reflections and interference. Finally, we implement a doping dependent optical thin-film simulation model. It enables us to precisely replicate the experimental luminance and angle-dependent emission spectrum for a range of LECs with different thicknesses. Using the model we can also identify and quantify many of the different optical loss mechanisms in LECs, which has not previously been done. The insights that we have collected on the path towards our present model will be useful for computational determination of device parameters that are otherwise difficult to acquire.The improved understanding of the optical operation of LECs is important for the maturation of the technology, as it facilitates formulation of relevant and accurate research questions. Hopefully, our results will accelerate the development of the field, so that useful products based on this technology can become available in the not too distant future.
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| 4. |
- Sandström, Robin, 1988-
(författare)
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Innovations in nanomaterials for proton exchange membrane fuel cells
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Hydrogen technologies are rapidly receiving increased attention as it offers a renewable energy alternative to the current petroleum-based fuel infrastructure, considering that continued large-scale use of such fossil fuels will lead to disastrous impacts on our environment. The proton exchange membrane fuel cell should play a significant role in a hydrogen economy since it enables convenient and direct conversion of hydrogen into electricity, thus allowing the use of hydrogen in applications particularly suited for the transportation industry. To fully realize this, multiple engineering challenges as well as development of advanced nanomaterials must however be addressed.In this thesis, we present discoveries of new innovative nanomaterials for proton exchange membrane fuel cells by targeting the entire membrane electrode assembly. Conceptually, we first propose new fabrication techniques of gas diffusion electrodes based on helical carbon nanofibers, where an enhanced three-phase boundary was noted in particular for hierarchical structures. The cathode catalyst, responsible for facilitating the sluggish oxygen reduction reaction, was further improved by the synthesis of platinum-based nanoparticles with an incorporated secondary metal (iron, yttrium and cobalt). Here, both solvothermal and high-temperature microwave syntheses were employed. Catalytic activities were improved compared to pure platinum and could be attributed to favorably shifted oxygen adsorption energies as a result of successful incorporation of the non-precious metal. As best exemplified by platinum-iron nanoparticles, the oxygen reduction reaction was highly sensitive to both metal composition and the type of crystal structure. Finally, a proton exchange membrane based on fluorine and sulfonic acid functionalized graphene oxide was prepared and tested in hydrogen fuel cell conditions, showing improvements such as lowered hydrogen permeation and better structural stability. Consequently, we have demonstrated that there is room for improvement of multiple components, suggesting that more powerful fuel cells can likely be anticipated in the future.
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| 5. |
- Auroux, Etienne, 1993-
(författare)
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Solution-processed light-emitting electrochemical cells : challenges and opportunities
- 2023
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Our world is filling up with electronics. High-tech gadgets are integrated everywhere, from smart fridges able to track expiry dates and food usage, to microchip implants that let us unlock doors and pay with our hands. As innovative as they are, these new products and the many more to come impose new requirements on materials and fabrication methods. For instance, emerging electronic technologies that deliver light emission such as smart labels, authenticity features and light-based medical therapies, are often required to be flexible, see-through and low-cost, and in addition sustainable to fabricate, operate and recycle.In response to these challenges, the light-emitting industry is turning to organic electronics for solutions, a field that promises resource-efficient fabrication using environmentally benign materials. An interesting proposal is that of the light-emitting electrochemical cell (LEC), which, thanks to its simple structure, is well suitedfor high-throughput fabrication. The LEC is in many aspects a smart device, able to reorganize itself during operation via the electrochemical action of mobile ions, which create the injection and transport layers that require additional fabrication steps in other technologies. This elegant behavior makes the LEC tolerant to a large array of materials and fabrication methods, and hence a good fit for many applications.Yet the LEC is still today a scientific curiosity rather than an actual commercial solution and among the very few prototypes available on the market, none are able to meet the combined performance, resource efficiency and sustainability criteria. As a matter of fact, of the three layers that make an LEC, i.e., two electrodes surrounding an active material, only the later meet these requirements thanks to a strong recent research effort. In comparison, the electrodes have received little attention and are almost exclusively comprising metals or metal oxides deposited by time- and energy-expensive fabrication methods, making the LEC as a whole unfit for many applications.In an effort to push the LEC toward the untapped commercial niche of low-cost lighting, we tackle the problem of electrode fabrication with resource-efficiency in mind. We first show that up-scalable spray coating of inks under ambient air is a viable mean of fabrication for both active materials and electrodes alike. However, in doing so, we find that we create electrode interfaces that are open to ion transfer; an up-to-now overlooked issue that needs careful consideration when designing solution-processed LECs. Building on our discovery, we demonstrate that it is possible to fabricate an LEC entirely by using spray coating metal-free and organic inks; thereby demonstrating that an all-organic, metal-free and resource-efficient LEC is possible.I hope that our efforts will encourage others to work on solution-processed LECs, electrodes included, and develop ready-to-use products.
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| 6. |
- Lundberg, Petter, 1988-
(författare)
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Light for a brighter morrow : paving the way for sustainable light-emitting devices
- 2020
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- We live in an artificially lit world, where light enhances our productivity and improves our quality of life. Today our appetite for light is stronger than ever, and emerging light-emitting technologies do not just replace the classical incandescent light bulb, they also open up for a new world of applications. The problem is that our environment does not cope with the increased energy demand during fabrication and usage, and the insufficient recycling that currently follows this rapid technological development. We must therefore adapt, and from here on out consider the entire environmental footprint and the necessity of our devices. Organic electronics has the potential to become sustainable. It allows for cheap and energy-efficient fabrication methods, using abundant materials, mainly carbon. Such sophisticated conductive plastics can be made thin and flexible, and they are thereby very versatile. It is in this context that we find the light-emitting electrochemical cell (LEC)—a strong contender for affordable and sustainable light. The LEC has a simple device design that is fit for solution based fabrication and new useful applications in, for example, medicine. The simple LEC design is enabled by its operational mechanism, where mobile ions aid electronic charge injection and improves electric conductivity by electrochemical doping. However, this dynamic nature complicates the attainment of devices that are efficient, bright, and retain a long lifetime. Herein, we face these challenges with sustainability as the beacon. We find that careful design of the active material, and selection of its constituents, can lead to LECs that are both efficient and bright. Importantly we show that this is attainable with entirely organic active materials, via thermally activated delayed fluorescence; thereby moving away from unsustainable phosphorescent emitters that contain problematic rare metals. With large-scale manufacturing in mind, we introduce a tool that identifies environmentally benign and functional solvents. Furthermore we design and validate a realistic optical model that unveils the common optical loss mechanisms in LECs. The insights gained guide the optical design of highly efficient LECs in the transition towards an upscaled production.I hope that the progress made will contribute to a road map for the design of sustainable light-emitting devices. It is then our responsibility, as a society, to make use of them where needed.
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