CoFe–N6 dual-atom sites enables the efficient generation of surface-bound ·OH for Fenton-like H2O2 activation

作者：Weidong Shang, Dongle Cheng, Longlong Zhang, Xiaoqiang Cao, Chongyang Ren, Huaqing Liu, Li Jie, Yanlong Wang, Zhijie Chen, Jian Zhang · 发表于：Applied Catalysis B: Environmental · 年份：2026 · DOI：10.1016/j.apcatb.2026.126837 · 被引用次数：2 · 研究领域：Electrocatalysts for Energy Conversion、Advanced battery technologies research、Advanced oxidation water treatment

Traditional Fenton processes are fundamentally limited by the inefficient generation and utilization of reactive ·OH species. Here, we engineer atomically dispersed Co–Fe pair sites anchored on biowaste-derived N-doped biochar (CoFe–N–BC), in a well-defined CoFe–N 6 coordination environment, enabling the selective generation of surface-bound ·OH (·OH surface ) and highly efficient Fenton-like oxidation. The catalyst achieves complete degradation of amoxicillin (AMX) in 20 min with a H 2 O 2 utilization efficiency of 99.7% and a rate constant of 0.238 min −1 . Quenching and electron paramagnetic resonance (EPR) results identify ·OH, particularly ·OH surface (accounting for 74% of all ·OH), as the dominant reactive species. The interaction of ·OH surface and porous biochar confines the catalytic reaction to the catalyst interface, inhibiting the ineffective self-quenching and side reactions of ·OH, promoting the utilization efficiency of ·OH. Further characterizations and density functional theory (DFT) calculations reveal that pyridinic N synergizes with Co/Fe to modulate the electron density, while the CoFe–N 6 motif lowers the H 2 O 2 activation barrier via a Co–O–N–O–Fe bridge, enabling continuous ·OH surface generation. Continuous flow tests demonstrate robust performance and stability in real wastewater, reducing operational costs by more than fivefold compared to conventional Fenton processes.