Electrochemical CO₂ reduction reaction (CO₂RR) has attracted a lot of interest as a highly potential CO₂ utilization system. Due to the high overpotential in CO₂RR, an effective catalyst is required. We report a metal-organic hybrid catalyst (Co-PPy-C), which consists of Co and polypyrrole, as a highly active electrocatalyst for CO₂RR. Co-PPy-C exhibited high Faradaic efficiency and metal mass activity for CO production at low overpotential region. By density functional theory calculations, it was revealed that the catalytic site is the Co surface on which the deprotonated pyrrolic functionality in polypyrrole is adsorbed, and that the facile production of CO from CO₂ is due to the CO adsorption on the Co being weakened by the charge transfer from the Co surface to the polypyrrole. This work reports a new and active non-noble metal catalyst for CO₂RR, and provides the strategy of hybridization of metal and organic material to modify or enhance the catalytic activity of metal for CO₂RR.

作为高潜力的CO ₂利用系统，电化学的CO ₂还原反应（CO ₂ RR）引起了人们的极大兴趣。由于CO ₂ RR中的超电势高，因此需要有效的催化剂。我们报告了一种金属有机混合催化剂（Co-PPy-C），它由Co和聚吡咯组成，作为CO ₂ RR的高活性电催化剂。Co-PPy-C在低超电势区域表现出高的法拉第效率和金属质量活性，可用于生产CO。通过密度泛函理论计算，发现催化位点是聚吡咯中去质子化的吡咯官能团被吸附的Co表面，并且由CO ₂容易产生CO这是由于从Co表面到聚吡咯的电荷转移削弱了Co在Co上的吸附。这项工作报告了一种新型的活性非贵金属催化剂，用于CO ₂ RR，并提供了金属和有机材料的杂化策略，以修饰或增强金属对CO ₂ RR的催化活性。