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C 2020, 6, 34 2 of 21 vision are highly desirable [16,17]. In this sense, some conversion routes are designed for the reuse of fuels, especially when inexpensive renewable energy processes are available. New approaches that transform CO2 in fine chemicals or value-added products are also being deeply investigating. The remunerability of the product is much higher and can economically support the development of the technologies involved. However, the volume of the potential market of these fine chemicals can hardly match with the volume of CO2 emissions, needing the development of a network of parallel CCU technologies. Hence, different strategies, including biological methods, have been developed either for directly producing reduced products (i.e., carbonic anhydrase, hydrogenation of CO2 to formate, reduction of CO2 to methane, CO2 conversion into methanol by enzyme cascade) or to store CO2 in biomass (e.g., algae) [18–20]. The photocatalytic reduction approaches also allow to synthetize a wide spectrum of CO2 reduction products, such as HCOOH, HCHO, CH3OH, or CH4, and can be effectively used by using visible responsive materials [21–27]. Adsorption, CO2 activation and further reduction to produce value-added products are crucial steps for photocatalytic processes. Sharma et al. reported a combined theoretical and experimental study describing the selective reduction of CO2 into methane through a robust visible-light photocatalyst based on single-phase ternary sulfide (CTS) [28]. Zhou et al. proposed the use of aqueous suspensions of cubic ZnS nanocrystals for the photocatalytic reduction of CO2 into formate [29]; and the development of heterostructures, such as Cu2O/TiO2, for artificial photosynthesis [30]. Chemical catalytic strategies for CO2 reduction have been proposed mainly based on the Sabatier reaction [31]. Finally, it is worthy to highlight that in the last years, it has been also reported that the development of electrochemical technologies to capture and transform CO2 into high-added value products is a suitable and green way for activating CO2 compared to others Carbon Capture, Utilization and Storage (CCUS) strategies [32]. Direct carboxylation of carbon nucleophile using CO2 as an electrophile is a straightforward route to prepare carboxylic acids. The main drawback associated to this process is related to the use of toxics reagents and the production of a large amounts of waste [33]. For instance, the conventional route for synthesizing 6-aminonicotinic acid from the corresponding nitriles involves low yields, hazardous chemicals (such as cyanide and ammonia gas) and high temperatures [34–36]. Nevertheless, using organic electrochemistry techniques improve environmental conditions [37–50]. One of the most widely used approaches for valorizing CO2, is to use organic halides with electrochemical techniques, which makes it possible to activate the CO2 (Scheme 1, Equations (1)–(4)); In a first step, a one electron transfer process generates the organic radical anion, which later converts to an anion though a second reduction electron transfer and a halide anion. The key to this approach relies on the reduction potential value of the organic halides and the stability of the organic anion formed after the reduction process [51–65]. The development of selective electrocatalysis processes for the reduction of carbon dioxide (CO2) to yield C1 products (such as CO (2e−), or higher Cn products) would allow the use of CO2 as a carbon feedstock (Scheme 1). Nevertheless, it is necessary to overcome high-energy barriers for the direct reduction of CO2, which commonly implies reduction potential values significantly more negative than the corresponding thermodynamic reduction potential value of CO2. In this sense, different types of electrodes have been studied for direct reduction of CO2. These cathodes are classified based on the nature of the main product obtained in the electrochemical process in aqueous and non-aqueous supporting electrolytes [66]. Moreover, it has also been developed other kinds of modified or doped electrodes (with immobilized enzymes, nanoparticles or metallic oxides) to catalyze CO2 direct reduction [67–69]. Hence, the improvement of electrocatalytic processes could lower overpotential requirements while maintaining appropriate catalytic rates and selectivity [70–91].PDF Image | Electrochemical Tuning of CO2 Reactivity in Ionic Liquids
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