Metal–organic frameworks (MOFs) with a large number of active sites and high porosity are considered to be good platforms for the carbon dioxide electroreduction reaction (CO₂RR) but with confined low conductivity or low efficiency. Here, Pd-[Bmim]PF₆/Cu-BTC with exceptional selectivity and electron-transfer ability is elaborately designed by introducing ionic liquids (ILs) into the MOFs. ILs favor promoting the overall current density of the catalysts, and the introduction of Pd atoms combined with O atoms on the catalyst surface reconfigures into strong Pd–O bonds, improving the desorption efficiency of *CO. The unique structure of the catalyst Pd-[Bmim]PF₆/Cu-BTC leads to a significant improvement of the C₁ product with a high Faraday efficiency (FE) of 99.36%, especially for carbon monoxide (CO) with an FE of 93.18% (−1.1 V_RHE). The exceptional performance of the catalyst is verified by density functional theory (DFT) calculations, and the reduction of the free energy required by *HOCO as a key intermediate for CO production was only 0.12 eV, providing new insights to improve the electrocatalytic performance of MOF-based materials for the CO₂RR. In this research, an effective and promising strategy that configures active sites by larger current density is proposed to enhance the efficiency of the CO₂RR.

中文翻译：

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偶联 [bmim]PF6 和 Pd NPs 调制的 MOF 基材料用于协同调节电催化 CO2 还原


具有大量活性位点和高孔隙率的金属-有机框架 （MOF） 被认为是二氧化碳电还原反应 （CO₂RR） 的良好平台，但受限于低电导率或低效率。在这里，通过将离子液体 （ILs） 引入 MOF 中，精心设计了具有卓越选择性和电子转移能力的 Pd-[Bmim]PF₆/Cu-BTC。IL 有利于提高催化剂的整体电流密度，并且在催化剂表面引入 Pd 原子与 O 原子结合，重新构形成强 Pd-O 键，从而提高 *CO 的解吸效率。催化剂 Pd-[Bmim]PF₆/Cu-BTC 的独特结构使 C₁ 产物得到显著改进，法拉第效率 （FE） 高达 99.36%，尤其是一氧化碳 （CO） 的法拉第效率 （FE） 为 93.18% （−1.1 V_RHE）。密度泛函理论 （DFT） 计算验证了催化剂的卓越性能，*HOCO 作为 CO 生产的关键中间体所需的自由能减少量仅为 0.12 eV，为提高 MOF 基材料的 CO₂RR 电催化性能提供了新的见解。在这项研究中，提出了一种有效且有前途的策略，通过更大的电流密度来配置活性位点，以提高 CO₂RR 的效率。