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sustainable production of fuels and chemicals

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to restructure under reaction conditions, negatively impacting performance over time. Studies of nanostructured catalysts have identified particle size, shape, roughness, defect density, and metal composition as the main factors that govern CO2RR activity and selectivity (Figure 2.3) [3–5]. Environmental conditions (e.g. local pH , electrolyte, electric fields) have also been found to play a crucial role in determining the CO2RR selectivity [5], but understanding many of these effects from a mechanistic perspective remains a challenge. Figure 2.3: Schematic of the parameters influencing the activity and selectivity of CO2RR catalysts. Reproduced with permission from [3] and [5]. Most current CO2RR studies are performed in H-type cells with CO2 dissolved in an aqueous electrolyte, which means the upper bound of the reaction rate is limited by the low solubility of CO2 regardless of catalyst performance. The field has begun moving closer to practical applications by studying complex electrode assemblies and cell designs that employ gas-diffusion electrodes and allow operation at industrially relevant current densities (>100 mA/cm2) [6]. The first multi-stack CO2 electrolysis cell has also been recently demonstrated [7]. 2.3 Future research needs For CO2RR to become competitive with the fossil fuel-derived industry, its energy efficiency, re- action rate, selectivity, and long-term stability should be comparable to water electrolysis. A longer-term goal is to advance these metrics for CO2RR to those of the thermal catalytic con- version processes considered in Sections 3 and 4. To reach these goals, the development of novel catalysts, suitable and stable membranes, electrolytes, gas-diffusion layers, and electrolysis cell ar- chitectures are key challenges. To this end, we propose five critical research areas that deserve attention in the near future. 2.3.1 Improving catalyst activity, selectivity, and stability Sufficient enhancements in energy efficiency require operating at significantly lower CO2RR overpo- tentials than the state of the art. For C1 products, cascade cell operation having CO as intermediate product would require achieving catalyst efficiencies of up to 70%. Different approaches can be un- 21

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