Graphdiyne interface engineering : highly active and selective ammonia synthesis

Abstract

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 (YNH3) and Faradaic efficiency (FE) of 219.72 μg h−1 mgcat.−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.