Cheng Banggui, Du Jiehao, Yuan Huiqing, Tao Yuan, Chen Ya, Lei Jingxiang, Han Zhiji
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
ACS Appl Mater Interfaces. 2022 Jun 22;14(24):27823-27832. doi: 10.1021/acsami.2c03748. Epub 2022 Jun 8.
Electrochemical CO reduction is a promising approach to obtain sustainable chemicals in energy conversion. Improving the selectivity of CO reduction toward a particular C product such as ethylene remains a significant challenge. Herein, we report a series of imidazolium hexafluorophosphate compounds as surface modifiers for planar Cu foils to boost the Faradaic efficiency (FE) of ethylene from 5 to 73%, which is among the highest reported using polycrystalline Cu. The modified electrodes are convenient to prepare. The structure-function study demonstrates that varying the alkyl or aromatic substituents on the imidazolium nitrogen atoms has significant effects on the morphology of the deposited films and the product selectivity of CO reduction. Experimental FE, FE, ln(FE/FE), and ln(FE/FE) values show generally linear relationships with FE while using different imidazolium modifiers, suggesting that factors governing proton reduction may also be directly related to both overall C generation and ethylene selectivity. This work presents an effective and practical way in tailoring the active sites of metallic surface for selective CO reduction.
电化学CO还原是一种在能量转换中获得可持续化学品的有前景的方法。提高CO还原对特定碳产物(如乙烯)的选择性仍然是一项重大挑战。在此,我们报道了一系列六氟磷酸咪唑鎓化合物作为平面铜箔的表面改性剂,将乙烯的法拉第效率(FE)从5%提高到73%,这是使用多晶铜报道的最高值之一。改性电极制备方便。结构-功能研究表明,改变咪唑鎓氮原子上的烷基或芳基取代基对沉积膜的形态和CO还原的产物选择性有显著影响。实验FE、FE、ln(FE/FE)和ln(FE/FE)值在使用不同咪唑鎓改性剂时通常与FE呈线性关系,这表明控制质子还原的因素可能也与总的碳生成和乙烯选择性直接相关。这项工作为定制金属表面的活性位点以实现选择性CO还原提供了一种有效且实用的方法。