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Abstract As an integrated CO 2 capture and utilization (ICCU) process, direct electrochemical reduction of amine captured-CO 2 reduction reaction (cCO 2 RR) has enormous advantages in energy efficiency and operating cost. The low product selectivity is an urgent issue. Here, we found that the hydroxyl (-OH) on CeO 2 can significantly enhance CO selectivity. After hydroxyl modification, the CO faraday efficiency (FE CO ) was surprisingly increased by 188% (relative increase rate). The correlation coefficient between -OH quantity and FE CO is as high as 0.98. Further study indicated that the presence of -OH can lead to a more compact electrochemical double layer (EDL) and charge transfer resistance by proton transfer. The -OH can also enhance CO 2 adsorption and stabilize the intermediate species (*COOH). DFT results further demonstrate that the rate-determining step was proton transfer from the surface -OH to MEACOO − , -OH modification can reduce the energy barrier to as low as 0.39 eV. This work provides additional insights into improving selectivity in amine-based cCO 2 RR, advancing the development of ICCU technology.
Wang et al. (Wed,) studied this question.