Active site engineering is of significant importance for developing high activity metal-organic frameworks (MOFs) for catalytic applications. Herein, we develop a one-pot strategy to construct bimetal organic frameworks with Fe-Co dual sites for Fenton-like catalysis. Density functional theory (DFT) demonstrated that the introducing Co heteroatoms into MIL-101(Fe) (MIL represents Matérial Institute Lavoisier) was favorable for the formation of electron-deficient centers around benzene rings and electron-rich centers around Fe/Co. This synergistic effect could effectively decrease the energy barrier of H₂O₂ activation. Due to the facilitated charge transfer in the coordinated structures, MIL-101(Fe,Co) with engineered dual sites exhibited exceptionally high efficiency for the degradation of ciprofloxacin (CIP). The reaction rate of MIL-101(Fe,Co)/H₂O₂ system was 0.12 min⁻¹, which was nearly 7.5 times higher than that of pristine MIL-101(Fe). The reaction mechanism of heterogeneous Fenton-like catalysis was fundamentally investigated by series of in-situ techniques, such as DRIFTS and Raman. ·OH radicals generated by H₂O₂ activation endowed the inspiring ability of MIL-101(Fe,Co) for water decontamination. This work offers a facile principle of exploring MOFs-based Fenton-like catalysts with a wide working pH range for environmental applications.

活动现场工程对于开发用于催化应用的高活性金属有机骨架（MOF）至关重要。在本文中，我们开发了一种一锅策略，以构建具有Fe-Co双位点的双金属有机骨架，以进行Fenton类催化。密度泛函理论（DFT）表明，将Co杂原子引入MIL-101（Fe）（MIL代表材料研究所Lavoisier）有利于在苯环周围形成缺电子中心，在Fe / Co周围形成富电子中心。这种协同作用可以有效降低H ₂ O ₂的能垒激活。由于协调结构中的电荷转移便利，具有工程双位点的MIL-101（Fe，Co）对环丙沙星（CIP）的降解表现出极高的效率。MIL-101（Fe，Co）/ H ₂ O ₂体系的反应速率为0.12 min ^-1，是原始MIL-101（Fe）的近7.5倍。通过一系列原位技术，如DRIFTS和Raman，从根本上研究了非均相Fenton类催化的反应机理。·H ₂ O ₂产生的OH自由基活化赋予了MIL-101（Fe，Co）净化水的启发能力。这项工作为探索基于MOF的，具有宽工作pH范围的Fenton类催化剂提供了简便的原理，适用于环境应用。