Coupling of N‐Doped Mesoporous Carbon and N‐Ti₃C₂ in 2D Sandwiched Heterostructure for Enhanced Oxygen Electroreduction

Abstract 2D heterostructures provide a competitive platform to tailor electrical property through control of layer structure and constituents. However, despite the diverse integration of 2D materials and their application flexibility, tailoring synergistic interlayer interactions between 2D materials that form electronically coupled heterostructures remains a grand challenge. Here, the rational design and optimized synthesis of electronically coupled N‐doped mesoporous defective carbon and nitrogen modified titanium carbide (Ti₃C₂) in a 2D sandwiched heterostructure, is reported. First, a F127‐polydopamine single‐micelle‐directed interfacial assembly strategy guarantees the construction of two surrounding mesoporous N‐doped carbon monolayers assembled on both sides of Ti₃C₂ nanosheets. Second, the followed ammonia post‐treatment successfully introduces N elements into Ti₃C₂ structure and more defective sites in N‐doped mesoporous carbon. Finally, the oxygen reduction reaction (ORR) and theoretical calculation prove the synergistic coupled electronic effect between N‐Ti₃C₂ and defective N‐doped carbon active sites in the 2D sandwiched heterostructure. Compared with the control 2D samples (0.87–0.88 V, 4.90–5.15 mA cm⁻²), the coupled 2D heterostructure possesses the best onset potential of 0.90 V and limited density current of 5.50 mA cm⁻². Meanwhile, this catalyst exhibits superior methanol tolerance and cyclic durability. This design philosophy opens up a new thought for tailoring synergistic interlayer interactions between 2D materials.