posted on 2023-12-06, 20:04authored byBoyang Li, Jinfang Kou, Gong Zeng, Jiantai Ma, Zhengping Dong
An ecofriendly and facile strategy
for converting aromatic
alcohols
to high-value-added compounds, especially acids and nitriles, is highly
desirable. Herein, atomically dispersed Co species anchored on N-doped
porous carbon were fabricated by simple one-pot pyrolysis using low-cost
precursors. The as-obtained Co/NC catalyst with a high Co loading
of 8.77 wt % exhibited excellent performance for the one-step oxidation
of aromatic alcohols. Under ambient air reaction conditions and with
the addition of KOH or NH3·H2O, the aromatic
alcohols were successfully converted to the corresponding aromatic
acids or aromatic nitriles, respectively. Experimental and theoretical
studies confirmed that the Co–N4 sites serve as
the primary active sites for the activation of aromatic alcohols.
The transformation of aromatic alcohols to aldehydes is a crucial
intermediate pathway. Density functional theory (DFT) calculations
revealed that compared to the Co nanoparticle catalysts, the Co/NC
catalyst with atomically dispersed active sites exhibited a lower
energy barrier for the aerobic oxidation of benzyl alcohol to benzaldehyde.
Additionally, the prepared single-atom Co/NC catalyst displayed remarkable
recyclability and applicability. This study provides not only a potential
strategy for constructing highly efficient non-noble metal catalysts
but also a facile approach for the aerobic oxidation of aromatic alcohols
to high-value-added products.