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C Journal of Carbon Research Article Electrochemical Tuning of CO2 Reactivity in Ionic Liquids Using Different Cathodes: From Oxalate to Carboxylation Products Silvia Mena and Gonzalo Guirado * Departament de Química, Universitat Autònoma de Barcelona, Campus UAB, 08193 Bellaterra, Spain; silvia.mena@uab.cat * Correspondence: gonzalo.guirado@uab.cat; Tel.: +34-93-581-4882 Received: 16 April 2020; Accepted: 21 May 2020; Published: 26 May 2020 Abstract: There is currently quite a lot of scientific interest in carbon dioxide (CO2) capture and valorization with ionic liquids (ILs). In this manuscript, we analyze the influence of the potential applied, the nature of the cathode and the electrolyte using different organic mediators, such as nitro or cyano aromatic derivatives, to promote the electrochemical activation of CO2. An electrocatalytic process using a homogeneous catalysis is seen when nitroderivatives are used, yielding to oxalate in organic electrolytes and ILs. Turnover frequency (TOF) values and Farafay efficiencies were slightly higher in N,N’-dimethylformamide (DMF) than in ILs probably due to the viscosity of the electrolyte. The use of cyano derivatives allows to tune the electrochemical reactivity in function of the reduction potential value applied from electrocarboxylated products (via a nucleophile-electrophile reaction) to oxalate. These electrochemical reactions were also performed using three different cathodes, organic electrolytes and ionic liquids. The use of copper, as a cathode, and ionic liquids, as electrolytes, would be a cheaper and greener alternative for activating carbon dioxide. Keywords: CO2; electrochemistry; ionic liquid; catalysis; carboxylation; green chemistry 1. Introduction Nowadays methane, nitrous oxide and carbon dioxide (CO2) emissions represents approximately 98% of the total greenhouse gas (GHG) inventory worldwide [1–3], and their share are expected to increase this twenty-first century. CO2 represents the most important GHG, which represents approximately the 77% of the global GHG emissions (considering its global warming potential) worldwide. Moreover, the change in atmospheric CO2 concentration has been considered the most important driver of global warming. In 2019 carbon dioxide emissions from energy stagnated at 33 Gt, which are mainly due to anthropogenic activities. Besides, it is expected to increase to 40.3 Gt by 2030 and to 50 Gt by 2050, if proper measures are not taken [4–7]. In the last decade, new concepts have been developed as a suitable approaches for facing the challenges of the current global scenario; so biomimetic [8] and circular economy models have been formulated. All the approaches involve a first capture step for an efficient removal of CO2 from common points sources prior to the release of gases into atmosphere [9–12]. Carbon capture and storage (CCS) approaches include planning the confinement of CO2 into depleted oil and gas wells, deep oceans, and aquifers [13]. Capture approaches based on chemical absorption and desorption using an aqueous amine solution are also one of the most promising option for separating CO2 from fossil-fuel-derived flue gas due to its simple operation, high absorption efficiency, cost-effectiveness and maturity [14,15]. However, all these strategies only partially solve the problem, so approaches to recover valuable products from its conversion through a circular economy C 2020, 6, 34; doi:10.3390/c6020034 www.mdpi.com/journal/carbonPDF Image | Electrochemical Tuning of CO2 Reactivity in Ionic Liquids
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