Ferrocene‐Based Nickel Metal–Organic Framework Nanosheets as Efficient, Long‐Cycle Cathode Catalyst for Li‐CO₂ Battery

Abstract Li‐CO₂ batteries, as a novel type of secondary battery, show great potential for energy conversion and storage. However, challenges such as large electrode polarization and poor cycling performance, stemming from difficulties in decomposing discharge products, limit their practical application. Here, Ferrocene‐based nickel metal–organic framework (Ni‐Fc) nanosheets structure to act as cathode catalysts, prepared via a one‐pot solvothermal reaction. X‐ray absorption fine structure (XAFS) analysis shows that Ni metal forms abundant catalytic active centers with O coordination of carboxylic acid groups in ferrocene units. The Ni‐Fc‐based battery demonstrates a high discharge capacity of 18636 mAh g⁻¹ and exhibits a cycle life exceeding 2000 h at a current of 200 mA g⁻¹. Density functional theory (DFT) calculations indicate that the stronger interaction of Ni‐Fc with discharge intermediates and enhanced Li adsorption accelerate battery reaction kinetics. This study introduces novel catalyst design concepts aimed at achieving high‐performance CO₂ reduction and oxidation, thereby advancing Li‐CO₂ batteries toward practical application.