Magnetic Core–Shell-Structured FeOx/CN Catalyst Mediated Peroxymonosulfate Activation for Degradation of 2,4-Dichlorophenol via Non-Radical Pathway,ACS ES&T Water

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Magnetic Core–Shell-Structured FeOx/CN Catalyst Mediated Peroxymonosulfate Activation for Degradation of 2,4-Dichlorophenol via Non-Radical Pathway
ACS ES&T Water ( IF 4.8 ) Pub Date : 2021-08-26 , DOI: 10.1021/acsestwater.1c00152
Kaijie Xu ₁ , Kangping Cui ₁ , Chenxuan Li ₁ , Minshu Cui ₁ , Rohan Weerasooriya _{2,

3} , Xiaoyang Li ₄ , Zhaogang Ding _{1,

2} , Xing Chen _{1,

2}

Affiliation

In this study, a magnetic nano-FeO_x/CN core–shell-structured catalyst with a high operating stability was successfully prepared by a coordinating polymer pyrolysis strategy. It exhibited high catalytic activity in peroxymonosulfate (PMS)-based advanced oxidation processes. Under neutral and room temperature conditions, the removal efficiency of 2,4-dichlorophenol (2,4-DCP) via FeO_x/CN/PMS system reached more than 90% within 60 min, and the removal of total organic carbon reached 89% within 90 min. The key operating parameters were evaluated and analyzed. Besides, in five consecutive degradation experiments, Fe-3/CN showed high stability, low iron ion loss, and excellent magnetic separation and recovery performance, demonstrating its potential as a practical Fenton-like catalyst. The abundant and orderly N pores in the CN structure provided key conditions for the anchoring and dispersion of nano-FeO_x particles. Electron paramagnetic resonance and free radical scavenging experiments proved that ¹O₂ is the main reactive oxygen species (ROS) that causes 2,4-DCP degradation (about 76.4% of the total contribution). Combined with density functional theory, the degradation pathway of 2,4-DCP was reasonably predicted. This study provides new ideas for the design and synthesis of Fenton-like catalysts with high stability and high activity.

中文翻译：

磁芯 – 壳结构的 FeOx/CN 催化剂介导的过硫酸盐活化通过非自由基途径降解 2,4-二氯苯酚

在这项研究中，通过配位聚合物热解策略成功制备了具有高操作稳定性的磁性纳米FeO _x / CN核壳结构催化剂。它在基于过一硫酸盐 (PMS) 的高级氧化过程中表现出高催化活性。在中性和室温条件下，FeO _x对 2,4-二氯苯酚 (2,4-DCP) 的去除效率/CN/PMS系统在60分钟内达到90%以上，总有机碳在90分钟内去除率达到89%。对关键操作参数进行了评估和分析。此外，在连续五次降解实验中，Fe-3/CN表现出高稳定性、低铁离子损失和优异的磁分离和回收性能，显示了其作为实用类芬顿催化剂的潜力。CN结构中丰富而有序的N孔为纳米FeO _x粒子的锚定和分散提供了关键条件。电子顺磁共振和自由基清除实验证明¹ O ₂是导致 2,4-DCP 降解的主要活性氧 (ROS)（约占总贡献的 76.4%）。结合密度泛函理论，合理预测了2,4-DCP的降解途径。该研究为高稳定性、高活性类芬顿催化剂的设计和合成提供了新思路。

更新日期：2021-10-08

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