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Iron-organic frameworks as effective fenton-like catalysts for peroxymonosulfate decomposition in advanced oxidation processes
npj Clean Water ( IF 10.4 ) Pub Date : 2023-05-06 , DOI: 10.1038/s41545-023-00251-z
Meng Li , Jiayu Song , Wei Han , King Lun Yeung , Shaoqi Zhou , Ce-Hui Mo

Although Fenton-like reactions have been extensively used to treat various organic contaminants in wastewaters (oily wastewaters, landfill leachate, denitrification with Fenton oxidized non-degradable large molecular organic pollutants, and removal of phosphorus, etc.), the difficulty in catalyst recovery and the instability of catalytic activity limit their practical application. Herein, iron atoms were inserted in a metal-organic framework (FeNC) with dual reaction sites as highly reactive and stable electro-Fenton-like catalysts for the catalytic oxidation of organic pollutants via the electro-Fenton-like activation reaction of peroxymonosulfate (PMS) with fractional leaching of metal ions. Experiments and density functional theory (DFT) calculations indicate that FeNC with FeN4 and Fe–Fe active sites can rapidly deliver electrons for PMS dissociation. Further, an electrolysis reactor was constructed for the on-site generation of reactive oxygen species, which can stably and continuously purify various organic wastewaters. The combined use of an electrolysis reactor and magnetic catalyst in the current study provides a direction for the long-term remediation of organic pollutants on an industrial scale.



中文翻译:

铁有机骨架作为高级氧化过程中过氧单硫酸盐分解的有效类芬顿催化剂

虽然类芬顿反应已被广泛用于处理废水中的各种有机污染物(含油废水、垃圾渗滤液、芬顿氧化不可降解大分子有机污染物反硝化、除磷等),但催化剂回收难度大和催化活性的不稳定性限制了它们的实际应用。在此,将铁原子插入具有双反应位点的金属有机骨架 (FeNC) 中作为高活性和稳定的类电芬顿催化剂,通过过氧单硫酸盐 (PMS) 的类电子芬顿活化反应催化氧化有机污染物) 与金属离子的分级浸出。实验和密度泛函理论 (DFT) 计算表明 FeNC 与 FeN 4和 Fe-Fe 活性位点可以快速为 PMS 解离提供电子。此外,还建造了电解反应器,用于现场产生活性氧,可以稳定、持续地净化各种有机废水。目前研究中电解反应器和磁性催化剂的联合使用为工业规模的有机污染物长期修复提供了方向。

更新日期:2023-05-07
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