| 3 | Hydrophobic perfluoroalkane modified metal‐organic frameworks for the enhanced electrocatalytic reduction of CO_(2)显示文摘The electrochemical reduction of CO_(2) to value‐added chemicals would be an efficient way to utilize CO_(2) and mitigate greenhouse gas emission.However,the associated competitive hydrogen evolution reaction(HER)in aqueous electrolytes usually leads to poor selectivity for the CO_(2) electroreduction reactions(CO_(2)RR).Due to their high specific surface areas and tunable single active sites,metal‐organic frameworks(MOFs)are considered as promising candidates for CO_(2)RR.Herein,the Fe‐porphyrin based Zr‐MOF,PCN‐222(Fe),was treated with perfluorocarboxylic acid to afford the hydrophobic Fn‐PCN‐222(Fe)(n=5 and 7,n is the number of fluorine atoms in the perfluoroalkyl chain)for improving the selectivity CO_(2)RR via inhibiting the HER.Owing to the single active Fe sites were positioned in a hydrophobic microenvironment,the optimal F5‐PCN‐222(Fe)shows a high Faradic efficiency of 97%toward production of CO at−0.7 V versus reversible hydrogen electrode.Meanwhile,F5‐PCN‐222(Fe)achieved a high turnover frequency value of 3850 h−1 at−0.8 V,which was almost 3.6 times higher than that of PCN‐222(Fe)and surpassed most of other reported MOFs.This study paves a new way to improve the selectivity of the CO_(2)RR via inhibiting the associated HER by increasing the hydrophobicity of the electrocatalysts. | Xu Yang Qiu‐Xia Li Shao‐Yi Chi Hong‐Fang Li Yuan‐Biao Huang Rong Cao | 2022 | SmartMat2022，3，1： | 1 |
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