Iron single-atom anchored N-doped carbon: An efficient catalyst for the one-pot, scale-up pentazolate synthesis

Abstract

The discovery of ambient stable pentazolate salts has paved the way a new frontier in pentazole chemistry, representing a distinctive category of energetic materials. One challenge impeding their practical applications lies in achieve scale-up the pentazolate synthesis via a facile and low-cost route. An efficient and recyclable iron single-atom catalyst with FeN₄ sites (Fe₁@NC-700) has been firstly developed by a pyrolysis-milling strategy for the scale-up pentazolate synthesis, achieving significant yields (38.4 g, 15% yield for NaN₅; 77.6 g, 26% yield for CoN₅) via a three-step, one-pot process with a low iron dosage (0.67 mol%). According to experimental and theoretical calculation results, the exceptional catalytic performance of Fe₁@NC-700 can be attributed to its stable FeN₄ enzyme-like catalytic active sites, which facilitate the formation of Fe(IV)=O intermediate, and can still maintains its catalytic activity even under weak acidic conditions and after 5 cycles.