Chen Cheng, Ji Runmei, Li Wei, Lan Yeqing, Guo Jing
College of Sciences, Nanjing Agricultural University, Nanjing, 210095, PR China.
China Tobacco Jiangsu Industrial Co., Ltd., Nanjing, 210019, China.
Chemosphere. 2023 Jun;326:138499. doi: 10.1016/j.chemosphere.2023.138499. Epub 2023 Mar 22.
In this study, iron-rich waste self-heating bag was reutilized as the raw material to prepare oxygen vacancies (OV) functionalized iron-based composite (iron oxide (FeO)-carbon-vermiculite, viz. OV-ICV), which exhibited excellent performance in the Fenton-like degradation of micropollutants via peroxydisulfate (PDS) activation. Above 95% of 1.0 mg/L carbaryl (CB) was efficiently eliminated in the presence of 0.1 g/L of OV-ICV and 0.5 mmol/L of PDS over a wide pH range of 3-10 within 30 min. Besides, OV-ICV also showed acceptable adaptability, stability, and renewability. Imbedding OV into FeO structure significantly generated more active iron sites and localized electrons, promoted the charge transfer ability, and assisted the redox cycle of ≡Fe(III)/≡Fe(II) for PDS activation. Mechanism investigation demonstrated that superoxide radicals (O) derived from the activation of molecular oxygen mediated the generation of HO, and both of them further enhanced the formation of more sulfate radicals (SO) and hydroxyl radicals (OH), which led to the efficient degradation and mineralization of CB. Furthermore, the degradation pathways of CB were proposed based on the intermediates identification. This work lays a foundation for the rational reutilization of iron-containing wastes modified with defect engineering in heterogeneous Fenton-like catalysis for the remediation of micropollutants wastewater.
在本研究中,富铁废自热袋被重新用作原料,以制备氧空位(OV)功能化的铁基复合材料(氧化铁(FeO)-碳-蛭石,即OV-ICV),该复合材料在通过过二硫酸盐(PDS)活化进行类芬顿降解微污染物方面表现出优异的性能。在0.1 g/L的OV-ICV和0.5 mmol/L的PDS存在下,在3 - 10的宽pH范围内,30分钟内可有效去除95%以上的1.0 mg/L西维因(CB)。此外,OV-ICV还表现出可接受的适应性、稳定性和可再生性。将OV嵌入FeO结构中显著产生了更多的活性铁位点和局域电子,促进了电荷转移能力,并辅助≡Fe(III)/≡Fe(II)的氧化还原循环以活化PDS。机理研究表明,分子氧活化产生的超氧自由基(O)介导了HO的生成,它们两者进一步促进了更多硫酸根自由基(SO)和羟基自由基(OH)的形成,从而导致CB的有效降解和矿化。此外,基于中间产物鉴定提出了CB的降解途径。这项工作为在非均相类芬顿催化中利用缺陷工程改性的含铁废物合理再利用以修复微污染物废水奠定了基础。