Lewis Acidity‐Enhanced Metal‐Organic Frameworks as High‐Efficiency Cathode Catalysts for Advanced Li‐CO₂ Batteries

Abstract Lithium‐carbon dioxide (Li‐CO₂) batteries have attracted significant attention as a potential solution to mitigate the greenhouse effect and meet the demand for high energy density storage systems. Designing efficient cathodic catalysts is crucial for the development of high‐performance Li‐CO₂ batteries. Herein, an innovative Lewis acidity‐enhancement strategy is proposed for the design of cathodic catalysts in Li‐CO₂ batteries. These results demonstrate that a metal‐organic framework (MOF) with stronger Lewis acidity exhibits a significantly lower overpotential of 1.27 V, compared to 1.58 V for the MOF with weaker Lewis acidity. The enhanced Lewis acidity of Mn3‐MOF accelerates both the CO₂ reduction reaction and lithium carbonate decomposition, leading to improved electrochemical performance, including better rate capability and cycling stability. This study emphasizes the critical role of Lewis acidity in the design of efficient catalysts and provides valuable insights for the development of high‐performance Li‐CO₂ batteries.