Atomically Dispersed Zn-Nx Sites in N-Doped Carbon for Reductive N-formylation of Nitroarenes with Formic Acid

Replacement of noble metal catalysts with low-cost, non-noble heterogeneous catalysts is highly desirable. Herein, we prepared a reactive, inexpensive and stable isolated single-atom Zn/N-doped porous carbon (ZnNC) catalyst derived from a versatile zeolitic imidazolate framework precursor. The optimized ZnNC-1000 with Zn-N-x species possesses high zinc loading (5.2 wt%) and nitrogen content (6.73 wt%), exhibits efficient catalytic performance in the one-pot N-formylation of nitroarene to the corresponding formamides by using formic acid as the hydrogen donor and formylation agent. H-2-D-2 exchange reaction and HCOOH-chemisorption experiments demonstrated that atomically dispersed Zn-N-x species are essential for the activation of hydrogen and HCOOH molecules, which finally contributed to the highest catalytic activity of ZnNC-1000 for the reductive N-formylation reaction.