Liu Wei, Zhai Pengbo, Li Aowen, Wei Bo, Si Kunpeng, Wei Yi, Wang Xingguo, Zhu Guangda, Chen Qian, Gu Xiaokang, Zhang Ruifeng, Zhou Wu, Gong Yongji
School of Materials Science and Engineering, Beihang University, Beijing, 100191, China.
College of Physics, Qingdao University, Qingdao, 266071, China.
Nat Commun. 2022 Apr 6;13(1):1877. doi: 10.1038/s41467-022-29428-9.
Electrochemical reduction of CO to multi-carbon fuels and chemical feedstocks is an appealing approach to mitigate excessive CO emissions. However, the reported catalysts always show either a low Faradaic efficiency of the C product or poor long-term stability. Herein, we report a facile and scalable anodic corrosion method to synthesize oxygen-rich ultrathin CuO nanoplate arrays, which form Cu/CuO heterogeneous interfaces through self-evolution during electrocatalysis. The catalyst exhibits a high CH Faradaic efficiency of 84.5%, stable electrolysis for ~55 h in a flow cell using a neutral KCl electrolyte, and a full-cell ethylene energy efficiency of 27.6% at 200 mA cm in a membrane electrode assembly electrolyzer. Mechanism analyses reveal that the stable nanostructures, stable Cu/CuO interfaces, and enhanced adsorption of the *OCCOH intermediate preserve selective and prolonged CH production. The robust and scalable produced catalyst coupled with mild electrolytic conditions facilitates the practical application of electrochemical CO reduction.
将二氧化碳电化学还原为多碳燃料和化学原料是一种减轻过量二氧化碳排放的有吸引力的方法。然而,已报道的催化剂总是表现出碳产物的法拉第效率低或长期稳定性差的问题。在此,我们报道了一种简便且可扩展的阳极腐蚀方法来合成富氧超薄氧化铜纳米板阵列,该阵列在电催化过程中通过自演化形成铜/氧化铜异质界面。该催化剂在使用中性氯化钾电解质的流动池中,对乙烯的法拉第效率高达84.5%,可稳定电解约55小时,在膜电极组件电解槽中,在200 mA cm² 时全电池乙烯能量效率为27.6%。机理分析表明,稳定的纳米结构、稳定的铜/氧化铜界面以及对*OCCOH中间体的增强吸附保持了选择性和延长的乙烯生成。这种稳健且可扩展制备的催化剂与温和的电解条件相结合,促进了电化学二氧化碳还原的实际应用。