Atomically Dispersed Co–S–N Active Sites Anchored on Hierarchically Porous Carbon for Efficient Catalytic Hydrogenation of Nitro Compounds
Guangji Zhang, Feiying Tang, Xin Wang, Liqiang Wang, You‐Nian Liu
Abstract
It is highly desired but challenging to develop non-noble metal-based hydrogenation catalysts that can replace noble metal-based ones for selective reduction of nitro compounds into amino compounds. Herein, we reported a hierarchically porous carbon-supported N,S dual-coordinated cobalt single-atom catalyst (Co1/NSC-AT) for hydrogenation of nitro compounds. The unique coordination environment of Co centers, combined with the hierarchically porous structure of carbon supports, endows Co1/NSC-AT with an excellent catalytic performance; the hydrogenation reaction can be efficiently performed under mild conditions (35 °C, ∼1bar H2) with high conversion and selectivity. The theoretical calculation reveals that the N,S dual-coordinated cobalt single-atom center (Co1S1N3) in Co1/NSC-AT acts as an active site for the hydrogenation reaction. Co1S1N3 possesses a lower reaction barrier for the rate-determining step than Co1N4 and Co nanoparticles. Moreover, N,S dual-coordinated environments can tailor the electronic structures of Co single atoms, which facilitate the desorption of H from the active sites, thus promoting the hydrogenation process.