Fe Single Atoms and Fe2O3 Clusters Liberated from N-Doped Polyhedral Carbon for Chemoselective Hydrogenation under Mild Conditions

In the area of catalysis, selective reduction of nitro compounds to amino compounds is a colossal challenge due to the existence of competitive reducible functional groups. Herein, an Fe-based catalyst Fe-SAs/Fe2O3ACs/N-doped polyhedral carbon (NPC) has been designed and synthesized. As we expected, compared with Fe-SAs and Fe-NPs, Fe-SAs/Fe2O3ACs/NPC shows excellent catalytic performance (turnover frequency up to 1923 h(-1), calculated with nitrobenzene), chemoselectivity, and tolerance during the hydrogenation reaction of nitro compounds under room temperature because of the synergistic effects between Fe-SAs and Fe2O3ACs. The theoretical calculations show that Fe-SAs prefers to undergo hydrazine decomposition to generate hydrogen and the Fe2O3ACs surface is more active toward the nitrobenzene reduction to aniline.