Sulfide enhances the Fe(II)/Fe(III) cycle in Fe(III)-peroxymonosulfate system for rapid removal of organic contaminants: Treatment efficiency, kinetics and mechanism
Sulfide enhances the Fe(II)/Fe(III) cycle in Fe(III)-peroxymonosulfate system for rapid removal of organic contaminants: Treatment efficiency, kinetics and mechanism
复制标题
硫化物增强 Fe(III)-过一硫酸盐体系中的 Fe(II)/Fe(III) 循环，快速去除有机污染物：处理效率、动力学和机制
DOI：
10.1016/j.jhazmat.2022.128970
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发表时间：
2022
影响因子：
13.6
通讯作者：
Qi Yang
中科院分区：
文献类型：
--
作者：
Kunjie Hou;Zhoujie Pi;Fei Chen;Li He;Fubing Yao;Shengjie Chen;Xiaoming Li;Haoran Dong;Qi Yang
Fe（II）或Fe（III）活化过一硫酸盐（PMS）用于环境净化受到Fe（III）转化为Fe（II）的低转化率的严重限制。在这里，我们发现这个令人困惑的问题实际上可以通过引入微量的S2-来解决。添加0.2 mM的S2-，PMS/Fe（III）体系对双酚A（BPA）的降解效率和总有机碳（TOC）的去除率分别提高了3.8倍和6.0倍。与此同时，秸秆和PMS利用率也分别显著提高了650%和160%。所构建的PMS/Fe（III）/S2-体系具有较宽的pH范围（3.2 ~ 9.5）和较强的抗腐殖酸、Cl-和NO3-能力。通过清除实验、电子顺磁共振测量、化学探针法和18 O同位素标记技术，确定了PMS/Fe（III）/S2-体系中的主要活性氧化剂物种。结果表明，FeIVO 2+是降解BPA的主要活性氧化剂，·OH、SO 4·-、O2·-和1 O2也参与了降解。最后，PMS/Fe（III）/S2-系统的通用性进行了评估，通过改变目标污染物，氧化剂，还原S物种。PMS/Fe（III）/S2-体系的构建为含S2-有机废水的处理提供了一些启示，从精炼厂和制革厂。
The activation of peroxymonosulfate (PMS) by Fe(II) or Fe(III) for environmental decontamination is severely limited by the low conversion rate from Fe(III) to Fe(II). Here, we found that this puzzling problem could virtually be solved by introducing trace amounts of S2-. With the addition of 0.2 mM S2-, the bisphenol A (BPA) degradation efficiency and total organic carbon (TOC) removal in PMS/Fe(III) system were improved by 3.8 and 6.0 times, respectively. Meanwhile, thekobsand PMS utilization efficiency also markedly increased by 650% and 160%, respectively. The constructed PMS/Fe(III)/S2-system exhibited a good applicability to a wide pH range (3.2 ~ 9.5) and high resistance to humic acid, Cl-and NO3-. The main reactive oxidant species in PMS/Fe(III)/S2-system were identified by scavenging experiments, electron paramagnetic resonance measurement, chemical probe approach, and18O isotope-labeling technique. The identification results revealed that FeIVO2+was the primary reactive oxidant species, while •OH, SO4•-, O2•-and1O2were also involved in the degradation of BPA. Finally, the generalizability of PMS/Fe(III)/S2-system was evaluated by varying the target pollutants, oxidants, and reducing S species. The construction of PMS/Fe(III)/S2-system provides some insights into the treatment of organic wastewaters containing S2-, e.g., from refineries and tanneries.