Novel Ionic Liquids For Electrochemical Applications

Abstract

This thesis is organized into three main sections, and is concerned with the design and synthesis of novel ionic liquids (ILs), and their associated electrochemical applications. In the first section, a general introduction to the field of ionic liquids is presented, followed by the synthesis and characterization details of all novel compounds used in the study. The second section summarizes work done on the development of more stable dye-sensitized solar cells (DSCs). An introduction to the field of photovoltaics and DSCs is first delivered in Chapter 3, which is followed by two chapters of original work on ionic liqiud-based electrolytes for DSC applications. In Chapter 4, it is shown that novel triazolium-based ionic liquids can be used to fabricate dye-sensitized solar cells, giving power conversion efficiencies of up to 6.00 %. The ionic liquid-based electrolytes are found to be compatible with a range of organic and inorganic photosensitizers, although the ruthenium-based dye (coded C106) exhibits the best performance. A device employing one of these newly-developed electrolytes is also shown to be very stable, retaining ca. 90% of its initial performance even after 1000 hours of continuous full sun illumination at 60 â—SC. In Chapter 5, we focus on the development of stable porphyrin-sensitized solar cells, using IL-based electrolytes. Our studies reveal that the long-term stability of porphyrin-based DSCs are highly dependent on additives in the electrolyte. In particular, it is found that the additive, guanidinium thiocyanate, is essential for the preparation of long-lived devices. It is also shown that the beneficial effect of this additive originates from the thiocyanate anion, rather than the guanidinium cation. The third section of this thesis deals with the ionic liquid-catalyzed electroi?Œchemical reduction of carbon dioxide. Following a general introduction on carbon dioxide mitigation using ionic liquids (Chapter 6), the results of our work in this area are presented in Chapter 7. Our studies reveal that not all ionic liquids are stable at the potentials required for CO2 reduction. However, the imidazolium-based salts generally perform quite well. The catalytic effect of the IL is found to mainly stem from the cation, with the anion playing a somewhat secondary role. Our results also demonstrate that substitutions on the imidazolium ring can have a huge impact on catalysis. Product analysis shows that the best-performing catalyst produces carbon monoxide as the dominant product, with Faradaic efficiencies of between 70 to 80 %.