Graphdiyne Interface Engineering: Highly Active and Selective Ammonia Synthesis

A freestanding 3D graphdiyne–cobalt nitride (GDY/Co₂N) with a highly active and selective interface is fabricated for the electrochemical nitrogen reduction reaction (ECNRR). Density function theory 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 atmospheric pressure and room temperature, the electrocatalyst creates a new record of ammonia yield rate (Y (Formula presented.)) and Faradaic efficiency (FE) of 219.72 μg h⁻¹ mg_cat. ⁻¹ and 58.60 %, respectively, in acidic conditions, higher than reported electrocatalysts. Such a catalyst is promising to generate new concepts, new knowledge, and new phenomena in electrocatalytic research, driving rapid development in the field of electrocatalysis.