content in solvent compositions, making it difficult to discriminate between these hypotheses and to properly assess the general function of the cations based solely on existing literature. Unraveling the underlying role of these cations in CO2 reduction performance holds the potential to open new avenues for the efficient design of non-aqueous electrochemical CO2 reduction systems. This thesis embarks on a comprehensive investigation into the influence of imidazolium cations on the performance of (predominantly) Au electrodes in the electrochemical reduction of CO2 in non-aqueous media. Rigorous measures have been taken to maintain anhydrous conditions, mitigating the potential interference from water (Chapter 2). Au electrodes were chosen as a benchmark catalyst facilitating a systematic exploration. The research strategy involves a combination of synthetic methodologies, electrochemical Figure 1.1. (a) Schematic representation of interactions involving imidazolium, as proposed by Kamet et al.3 This includes cation coordination with adsorbed intermediates, carboxylation, and a side reaction leading to oxalate formation as a byproduct on a Pd electrode. (b) Proposed mechanism by Lau et al.8 involving hydrogen bonding to adsorbed *CO2 intermediate as the main mechanism for C2-methylated imidazolium on Ag electrode. These studies were conducted in an acetonitrile environment. a b
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