Unsymmetrically N, S-coordinated single-atom cobalt with electron redistribution for catalytic hydrogenation of quinolines

Engineering unsymmetrical coordination is an efficient strategy for improving the performance of carbon supported single-atom catalysts for diverse applications. However, the exploration of this strategy to pre-pare carbon supported single-atom catalysts for hydrogenation reaction is still in infancy, especially for hydrogenation of quinolines. Herein, we report a protein-metal-ion-network strategy for preparation of single-atom cobalt supported on hierarchically porous carbon (SA-Co/NSPC). SA-Co/NSPC features unsymmetrically N/S-coordinated metal center, i.e., Co1-N3S1. Moreover, the carbon matrices possess an ultra-thin two-dimensional morphology and hierarchically porous structures. SA-Co/NSPC catalyst with Co1-N3S1 active site exhibits excellent catalytic performance for hydrogenation of N-heterocycles. The DFT calculation results show that the site of Co1-N3S1 reveals a significant electron redistribution in comparison to the Co1-N4, leading to a lower H* diffusion barrier and quinoline hydrogenation reaction barrier. SA-Co/NSPC catalyst combined with the unique hierarchically porous structure and high active Co1-N3S1 owns extraordinary catalytic performance for hydrogenation of quinolines.(C) 2022 Elsevier Inc. All rights reserved.

Automated summary

Engineering unsymmetrical coordination is an efficient strategy for improving the performance of carbon supported single-atom catalysts. In this study, a protein-metal-ion-network strategy was used to prepare a single-atom cobalt catalyst for hydrogenation of quinolines. The catalyst exhibited excellent catalytic performance due to its unsymmetrically N/S-coordinated metal center and hierarchically porous carbon matrices.