Enhanced treatment of high chloride organic wastewater under lower peroxymonosulfate consumption: A pathway for the formation of Fe(IV)=O excited by chloride ions

Applied Catalysis B: Environment and Energy Pub Date : 2024-08-08 DOI:10.1016/j.apcatb.2024.124471

Xianjing Liu, Ying Wang, John Crittenden, Qi Su, Huatao Mo

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Abstract

The inhibition of oxidation efficiency and the formation of toxic chlorinated organic byproducts owing to Cl still represent a significant threat to the treatment of high chloride organic wastewater using advanced oxidation processes. This study explores new pathways for utilizing Cl to promote the formation of Fe(Ⅳ)=O by single atom Fe-CNs catalysts under peroxymonosulfate (PMS) system, which significantly increases sulfamethoxazole (SMX) degradation rate constant by 2.97 times, enhances PMS utilization efficiency (reducing by 92 % PMS consumption) and simultaneously avoids the formation of chlorinated organic byproducts. Experiments and theoretical calculation revealed that the in-situ generated HClO (generated via the reaction of PMS and Cl) more easily reacts with Fe–pyridinic N active sites of Fe-CNs catalysts to generate Fe(Ⅳ)=O through a lower-energy-barrier pathway, rather than directly oxidates pollutants. This study provides an approach to utilize omnipresent Cl achieving high efficiency, high selectivity, low PMS consumption and harmless treatment for chloride-containing organic wastewaters.

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在降低过一硫酸盐消耗量的情况下加强对高氯化物有机废水的处理：氯离子激发的 Fe(IV)=O 的形成途径

Cl 对氧化效率的抑制和有毒氯化有机副产物的形成仍然是使用高级氧化工艺处理高氯化物有机废水的重大威胁。本研究探索了单原子 Fe-CNs 催化剂在过一硫酸盐（PMS）体系下利用 Cl 促进 Fe(Ⅳ)=O 形成的新途径，使磺胺甲噁唑（SMX）降解速率常数显著提高 2.97 倍，提高了 PMS 利用效率（减少了 92% 的 PMS 消耗），同时避免了氯化有机副产物的形成。实验和理论计算表明，原位生成的 HClO（通过 PMS 和 Cl 反应生成）更容易与 Fe-CNs 催化剂的 Fe 吡啶 N 活性位点反应，通过较低能障途径生成 Fe(Ⅳ)=O，而不是直接氧化污染物。这项研究提供了一种利用无处不在的 Cl 实现高效率、高选择性、低 PMS 消耗和无害化处理含氯化物有机废水的方法。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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Applied Catalysis B: Environment and Energy

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