Development and Mechanistic Study of Single Sites in 2D-Covalent Organic Frameworks for Co2 Electroreduction

Identifier:  TDX:4172

Handle: https://hdl.handle.net/20.500.11797/TDX4172

Authors:  Dubed Bandomo, Geyla Caridad

Abstract:
Global warming, climate change and our over-dependence on non-renewable fossil fuels demand long-term solutions to reduce CO2 emissions and develop sustainable energy technologies. The electrochemical CO2 reduction has the potential to accomplish a “carbon-neutral energy cycle”, which incorporates CO2 as the unlimited carbon source for the production of high-density fuels. However, for an industrial application, there are still challenges to overcome, such as low selectivity, short durability and low current densities along with high overpotentials. New sustainable, modular, robust and efficient catalytic platforms are needed. In this regard, this PhD dissertation entails a fundamental understanding of the CO2 mechanisms using Single Atom Catalyst within Covalent Organic Frameworks (COFs). This thesis focuses on the investigation of the electrochemical CO2 reduction using new Manganese based-COFs with emphasis on understanding the relationship between structure and electrocatalytic activity. The initial center of interest of this work is to accomplish active performance and durability for CO2 reduction using highly-organized {Mn(CO)3} active sites within COFs. Compared to equivalent Mn derivates, COFs exhibited higher selectivity and activity.