Graphical Abstract

As a carbon-neutral alternative to the Haber-Bosch process, electrochemical N2 reduction enables environment-friendly NH3 synthesis at ambient conditions but needs active electrocatalysts for the N2 reduction reaction. Here, we report that conductive metal-organic framework Co3(hexahydroxytriphenylene)2 (Co3HHTP2) nanoparticles act as an efficient catalyst for ambient electrochemical N2-to-NH3 fixation. When tested in 0.5 M LiClO4, such Co3HHTP2 achieves a large NH3 yield of 22.14 μg·h-1·mg-1cat. with a faradaic efficiency of 3.34% at -0.40 V versus the reversible hydrogen electrode. This catalyst also shows high electrochemical stability and excellent selectivity toward NH3 synthesis.