Summary The combustion of carbon-based fuels has led to the persistent accumulation of carbon dioxide (CO2) in the Earth's atmosphere, resulting in far-reaching climate changes. To address this pressing global issue, there is an urgent need for sustainable and efficient methods to harness CO2 as an energy source, thus mitigating its environmental impact. One of the most promising approaches for CO2 utilization is electrochemical reduction, often carried out in water due to its green and abundant nature. However, the intrinsic electrochemical reactivity of water presents challenges in this process This PhD thesis explores the potential for improving carbon dioxide (CO2) reduction efficiency by transitioning from water-based electrochemical processes to non-aqueous media, using acetonitrile as a solvent. To enhance efficiency, imidazolium cations are introduced as cocatalysts and essential components of the electrolyte. The central aim of this work is to gain a fundamental understanding of the pivotal role of imidazolium cations in promoting nonaqueous electrochemical CO2 reduction. Additionally, it investigates their potential in facilitating efficient electrochemical conversion across a variety of affordable transition metals. By analyzing the structure-activity relationship for imidazolium electrolyte cations, this research provides insights into the selection or synthesis of effective electrolyte cations to enhance non-aqueous electrochemical CO2 reduction.
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