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Rapid oxidation of 4-cholorphenol in the iron-based Metal–Organic frameworks (MOFs)/H2O2 system: The ignored two-steps interfacial single-electron transfer
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2022-01-04 , DOI: 10.1016/j.seppur.2021.120420
Yi Han 1 , Mingjie Huang 1, 2 , Wei Xiang 1 , Chen Wang 1 , Yongjie Li 1 , Xiaohui Wu 1 , Juan Mao 1 , Tao Zhou 1 , Hong Li 3 , Deming Wu 3
Affiliation  

Fe-based metal–organic frameworks (MOFs) are popular in activating oxidants e.g·H2O2 and persulfate (PS) for degrading recalcitrant organic substances, generally regarded with a simple interfacial efficient iron cycle. This study has revealed that a novel two-steps single-electron transfer mechanism would occur initially to activate the rapid degradation 4-chlorophenol (4-CP) in the MIL-88B(Fe)/H2O2 system (88B/H2O2 system). The degradation of 4-CP was acidic favorable (pH0 ≤ 6.0) and could be divided into two reaction stages, i.e., initial lag phase (0–10 min) and following rapid decay phase (10–50 min). In the first stage, H2O2 was slowly activated on the surface of 88B to form superoxide radical (O2•–), which would lead to the accumulation of the key intermediate hydroquinone (HQ) through reducing 4-CP. Afterwards, HQ could reductively dissolve iron ions which would lead to the subsequent efficient homogeneous Fenton reaction for the rapid oxidation of 4-CP by hydroxyl radical (•OH) in the following rapid decay phase. It was interesting to note that specific aromatic compounds, which would form reductive benzenediols intermediates by O2•–, could be efficiently degraded in the 88B/H2O2 system. The result of this study is expected to provide a new insight for understanding the catalytic oxidation process based on MOFs, and its application if possible.



中文翻译:

铁基金属-有机框架 (MOFs)/H2O2 体系中 4-氯酚的快速氧化:被忽略的两步界面单电子转移

铁基金属有机骨架 (MOF) 在活化氧化剂如·H 2 O 2和过硫酸盐 (PS) 中很受欢迎,用于降解顽固的有机物质,通常被认为具有简单的界面有效铁循环。该研究表明,最初会出现一种新的两步单电子转移机制,以激活 MIL-88B(Fe)/H 2 O 2系统 (88B/H 2 ) 中的快速降解 4-氯苯酚 (4-CP) O 2系统)。4-CP 的降解呈酸性(pH 0  ≤ 6.0),可分为两个反应阶段,即初始滞后阶段(0-10 分钟)和随后的快速衰减阶段(10-50 分钟)。在第一阶段,H 2 O2在88B表面缓慢活化形成超氧自由基(O 2 •– ),通过还原4-CP导致关键中间体对苯二酚(HQ)的积累。之后,HQ 可以还原溶解铁离子,这将导致随后的高效均相 Fenton 反应,在随后的快速衰减阶段中,羟基自由基 (•OH) 快速氧化 4-CP。有趣的是,可以通过 O 2 •–形成还原性苯二醇中间体的特定芳族化合物可以在 88B/H 2 O 2中有效降解系统。这项研究的结果有望为理解基于 MOFs 的催化氧化过程及其应用提供新的见解。

更新日期:2022-01-20
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