Sobhan Neyrizi

 Perspectives An intriguing feature that awaits resolution in future investigations is the subtle distinction in the promotional impact of imidazolium cations and alkali metals. Considering the results from this thesis and drawing insights from previous endeavors, we can now propose that both categories of cations play a pivotal role in promoting CO2 reduction by providing essential solvation/stabilization for the negatively charged *CO2 - intermediate. While this thesis has expounded upon the hydrogen bonding as primary source of the promotional effect for C2 hydrogenated cations, alkali metals have been argued to promote the reaction through shortrange electrostatic interactions. The difference in the nature and the extent to which they efficiently stabilize the *CO2 - intermediate holds theoretical and experimental interest for future study. Throughout this thesis, we meticulously investigated the performance of imidazolium cations in dry acetonitrile, with occasional deviations due to unavoidable atmospheric exposure. While our efforts maintained relatively dry conditions, which correlated with the observed 100% faradaic efficiency for CO formation, a critical consideration arises when desiring altered selectivity for hydrogenated products. This shift necessitates the presence of proton donors in the system. Remarkably, inadvertent water introduction to the experimental setup led to the unexpected observation of ethanol as a product during experiments with a Ni electrode in the presence of water within MM-acetonitrile electrolytes (see Appendix Section A.I). Although requiring further validation, this observation implies the potential manipulation of product outcomes within imidazolium-acetonitrile electrolytes through controlled addition of proton donors. The impact of water on product selectivity has also been highlighted in prior work by Mendieta-Reyes et al.119 Their findings revealed the emergence of methanol on TiO2 electrodes in acetonitrile containing 0.5 M water, highlighting the potential role of water as a moderator in the selectivity landscape.

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