Carbon dioxide capture and utilization technologies are necessary to create a truly circular economy. The electrochemical reduction of carbon dioxide to formate is an appealing carbon utilization... Show moreCarbon dioxide capture and utilization technologies are necessary to create a truly circular economy. The electrochemical reduction of carbon dioxide to formate is an appealing carbon utilization method as it can be performed at room temperature and pressure, it only requires two electrons, and it has a high atom efficiency. This reaction has been known and studied for decades, but no commercial process is currently practiced.This thesis reviews work that has been performed in the field of electrocehmical reduction of CO2 toward formate and reviews how a gas diffusion electrode functions. A gas diffusion layer production method is explored for ways to tune the characteristics of the gas diffusion layer. A design of experiments is used to explore how the catalyst layer can interact with the gas diffusion layer. The best results (100% CE at 400mA/cm2) are scaled-up from 10 cm2 to 200 cm2. Contaminants in an industrial CO2 stream are studied using density funcitonal theory to determine their potential to poison electrocatalysts known to convert CO2 to formate. Show less
Heterogeneous catalysis is essential to many industrial applications. These catalysts are often comprised of supported nanoparticles, which contain various different surface sites. For some... Show moreHeterogeneous catalysis is essential to many industrial applications. These catalysts are often comprised of supported nanoparticles, which contain various different surface sites. For some reactions, the presence of specific surface sights dominates the overall reactivity. Fundamental insight into the influence of different surface sites on the surface reaction dynamics may lead to better catalyst design in the future. In this thesis, we combine ultra-high vacuum techniques and (curved) single crystal surfaces to study surface structure effects relevant to heterogeneous catalysis. We study how step edges on a platinum surface affect (elementary) reactions that occur in oxygen reduction: hydrogen dissociation, hydrogen recombination, and oxygen reduction. Show less
The thesis has shown that the metal porphyrin complexes are effective catalysts for both the electrochemical reduction of carbon dioxide and nitrate. pH plays an important role on both the... Show moreThe thesis has shown that the metal porphyrin complexes are effective catalysts for both the electrochemical reduction of carbon dioxide and nitrate. pH plays an important role on both the electroreduction of carbon dioxide and nitrate. The insights into the mechanism for both reactions offer the opportunity for the design of new effective catalysts in the future. Show less