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dertaken in order to develop more active and selective CO2RR electrocatalysts, including tuning the catalyst surface morphology, surface composition, and interaction with the electrolyte. Hy- brid approaches combining heterogeneous and molecular catalysts may be especially interesting for improving selectivity. An important aspect of improving selec- tivity towards carbon products requires quench- ing the hydrogen evolution reaction (HER), which concurrently takes place under CO2RR conditions. Additionally, the selective produc- tion of any single multi-carbon product is rarely achieved. Overcoming these challenges necessi- tates a better understanding of the roles of pH gradients near the electrode surface, mass trans- port, local buffering capacity, electrode charge, and local mesoscale electrode architecture on the overall performance of porous, high surface area electrodes. If sufficiently selective catalysts for particular products remain elusive, the inte- gration of efficient separation technologies may be needed. Towards improving stability, a deeper un- derstanding of the dynamic evolution of elec- trode structure and surface composition at the atomic-scale is necessary. Control of catalyst structure for thousands of hours of CO2RR op- eration is already an immense challenge that will only be enhanced once intermittent operation due to renewable energy sources is considered. In general, the stability of electrode surfaces under large cathodic overpotentials (“cathodic corrosion”) is relatively unexplored and needs to be addressed at a more fundamental level, combining theory and experiment (Figure 2.4). Figure 2.4: (a) Operando EC-AFM images of Cu cubes ac- quired in 0.1 M KHCO3 at open circuit potential (OCP) and at –1.1 V vs RHE for 1 min. (b) EXAFS data of these samples acquired in air, in the electrolyte under OCP and operando af- ter 1 h CO2RR at -1 V vs RHE. (c) Temporal evolution of the faradic efficiency for CO2RR and HER of Cu Cubes (-1 V vs RHE). Adapted with permission from [8]. 2.3.2 Advancing fundamental understanding of CO2RR: in situ techniques Many of the major challenges in this field arise from the general lack of fundamental understanding of the reaction mechanism for the most active and complex catalysts, hindering the design of improved electrode/electrolyte systems. To rationally design an efficient catalyst, one must be able to evaluate candidates under realistic reaction conditions. Along these lines, the development of improved in situ and operando microscopic and spectroscopic characterization techniques is 22PDF Image | sustainable production of fuels and chemicals
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