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Assessment of new catalysts for electrochemical reduction of carbon dioxideGoel, Ekta 09 August 2019 (has links)
The industrial revolution caused the release of carbon dioxide (CO2) into the atmosphere leading to a climate crisis. The impact of more CO2 in the atmosphere has been experienced by everybody. The summers are longer and hotter, while the winters are colder and shorter. The ocean water has become more acidic threatening the ocean life. There is an immediate need to reduce CO2 and switch to alternate energy for human survival. Electrochemical reduction of CO2 (ERC) is a promising technology capable of converting excess CO2 into valueded products. The process of recycling CO2 can address the problem of excess CO2 and is a sustainable solution until our dependence on fossil fuels is reduced. However, currently there are very few catalysts that can convert CO2 into valuable products with a low overpotential. The current research evaluates new catalysts for their ERC potential. [Ni(cyclam)]2+ is a well-known catalyst used to reduce CO2 homogeneously. Therefore, it was used as a standard to optimize the CO2 evaluation protocol. Two new catalysts developed in Dr. Hollis's laboratory, a Pt- pincer and a Fepincer molecule were assessed using this method. Cyclic voltammetry and bulkelectrolysis (BE) experiments were performed under Ar and CO2 environments. The gaseous products from BE were primarily CO and H2 and their quantitative measurement was performed using gas chromatography. Formate determination was performed using UV-Vis spectroscopy. Faradaic yields were calculated for CO, H2, and formate. The overpotentials were calculated for all the processes, and a comparison was made to determine the most efficient process. The turnover numbers (TON) and the turnover frequencies (TOF) of all the catalysts were calculated. Based on all the criteria, the Fepincer complex was determined to be the most promising catalyst for further optimization. Additionally, a Faradaic efficiency calculation spreadsheet was created to improve calculation efficiency. The protocol described here has been successfully applied to assess new catalysts and can prove to be an invaluable tool when numerous catalysts require evaluation.
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