Development and Mechanistic Analysis of Novel CO2 Reduction Electrocatalysts
Date
2023-01-13
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Abstract
The ever-growing anthropogenic concentrations of CO2 in our atmosphere has led to an entire industry centered around Carbon Capture and Utilization (CCU). One central pillar of the CCU ideology is the conversion of captured CO2 to “value-added” products such as carbon monoxide, formic acid, or commercial products such as plastics or vodka. However, the technologies that this industry rely on are not robust with suspect surface characterization and transient catalytically active sites. Solution phase molecular electrocatalysts are inherently impractical for industrial-scale CO2 conversion due to several complicating factors. However, the insights and knowledge developed from these homogeneous systems can often be directly utilized within industrial-scale heterogeneous electrolyzers with dramatic improvements to catalytic efficacy. Therefore, through the study of homogeneous systems, significant progress can be potentially made towards the effective valorization of CO2. With this in mind, the research outlined in this thesis details the development, exploration and mechanistic analysis of a range of novel CO2RR electrocatalysts with a special focus on earth abundant systems. Using ligand design principles developed through the literature, novel ligands were explored and CO2 reduction capabilities investigated. Once a promising target was identified, an intense mechanistic analysis was undertaken using spectroelectrochemistry and chemical reduction studies to identify and characterize key intermediates in the catalytic cycle. Through this analysis we have confirmed ideas on the importance of redox non-innocent ligands and developed new design principles centered around structural torsional strain. These insights provide value to developing next generation CO2RR electrocatalysts.
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Keywords
Electrocatalysis, Carbon Dioxide, Mechanism
Citation
Dubrawski, Z. S. (2023). Development and mechanistic analysis of novel CO2 reduction electrocatalysts (Doctoral thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca.