Ultrathin Co3O4 Layers Realizing Optimized CO2 Electroreduction to Formate

Electroreduction of CO₂ into hydrocarbons could contribute to alleviating energy crisis and global warming. However, conventional electrocatalysts usually suffer from low energetic efficiency and poor durability. Herein, atomic layers for transition‐metal oxides are proposed to address these problems through offering an ultralarge fraction of active sites, high electronic conductivity, and superior structural stability. As a prototype, 1.72 and 3.51 nm thick Co₃O₄ layers were synthesized through a fast‐heating strategy. The atomic thickness endowed Co₃O₄ with abundant active sites, ensuring a large CO₂ adsorption amount. The increased and more dispersed charge density near Fermi level allowed for enhanced electronic conductivity. The 1.72 nm thick Co₃O₄ layers showed over 1.5 and 20 times higher electrocatalytic activity than 3.51 nm thick Co₃O₄ layers and bulk counterpart, respectively. Also, 1.72 nm thick Co₃O₄ layers showed formate Faradaic efficiency of over 60 % in 20 h.