Efficient dinitrogen fixation on porous covalent organic framework/carbon nanotubes hybrid at low overpotential

Electrocatalytic nitrogen reduction under ambient conditions is a promising approach for ammonia synthesis, but it is challenging to develop highly efficient electrocatalysts. In this work, a hybrid of covalent organic framework (COF) and carbon nanotubes (CNTs) are developed for efficient nitrogen electroreduction with a high faradaic efficiency (FE) of 12.7% at 0.0 V versus reversible hydrogen electrode (RHE) and a remarkable production rate of ammonia up to 8.56 [Formula: see text]g h[Formula: see text] mg[Formula: see text] at –0.2 V versus RHE. Experiments and theoretical calculations reveal that Ni centers are active sites for NH 3 synthesis, while the [Formula: see text]–[Formula: see text] stacking between COF-366-Ni and conductive CNTs scaffold results in the rapid interfacial charge transfer. This investigation provides new insights on the rational design of organic–inorganic porous hybrids for efficient nitrogen conversion and ammonia synthesis at ambient conditions.