Graphdiyne interface engineering: highly active and selective ammonia synthesis

A freestanding 3D graphdiyne-cobalt nitrides (GDY/Co 2 N) with highly active and selective interface is fabricated for electrochemical nitrogen reduction reaction (ECNRR). Density function theory (DFT) calculations reveal that the interface bonded GDY contributes an unique p-electronic character to optimally modify the Co-N compound surface bonding, which generates as-observed superior electronic activity for NRR catalysis at the interface region. Experimentally, at the atmospheric pressure and room temperature, the electrocatalyst creates a new record of ammonia yield rate (Y NH3 ) and Faradaic Efficiency (FE) of 219.72 mug h -1 mg cat. -1 and 58.60 %, respectively, in acidic conditions, higher than reported electrocatalysts. Such catalyst is promising to generate new concepts, new knowledge, and new phenomena in electrocatalytic research, driving rapid development in the field of electrocatalysis.