experiments, and Density Functional Theory (DFT) calculations aimed at providing deep insights into the promotional effect that imidazolium cations exert on CO2 reduction. In particular, the influence of substituents at both C1, C3- and at the N1, N3- positions of the imidazolium ring on its catalytic performance will be scrutinized (Chapters 3 and 4). This analysis will shed light on the structure-activity relationships governing the impact of cations on CO2 reduction. Expanding the investigation, the performance of anhydrous imidazoliumacetonitrile will be systematically examined on other electrode materials, including Ag, Zn, Cu, and Ni (Chapter 5). This broader exploration aims to understand the generality of the observed effects and the potential for cation-mediated enhancement across different catalysts. Furthermore, the performance of C2-methylated imidaozlium cation will be investigated using in-situ FTIR spectroscopy (Chapter 6). Finally, the impact of the alkyl chain length of 1-alkyl3-methyl imidazolium cations on their catalytic efficiency will be also discussed (Chapter 7).
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