铁硫掺杂碳纳米材料活化过硫酸盐降解磺胺甲 唑

doi:10.19965/j.cnki.iwt.2024-0579

摘要/Abstract

摘要：

非均相铁基材料因具有效果显著、成本较低等优点被广泛应用于活化过一硫酸盐（PMS）降解有机污染物，而如何有效促进催化剂中Fe²⁺/Fe³⁺循环从而提升其活化性能一直是研究的重点。以卡拉胶作为天然的S源和C源，采用一步煅烧法制备了铁硫碳纳米材料（Fe-SC-x），通过扫描电镜和X射线衍射等表征手段分析了Fe-SC-x的微观形貌及物质组成，并将其应用于活化PMS降解抗生素污染物磺胺甲唑（SMX），以评估其催化性能。结果表明，在900 ℃下制备的催化剂Fe-SC-900催化效果最佳，其活化PMS在40 min时可降解99.8%的SMX。此外，Fe-SC-900/PMS体系能够抵抗共存阴离子和天然有机质，具有良好的实际应用潜力。降解机理实验表明，·OH、SO₄ ^·-、O₂ ^·-和¹O₂均存在于Fe-SC-900/PMS体系中，且¹O₂和SO₄ ^·-对SMX的降解起主导作用。

关键词: 高级氧化, 过一硫酸盐, 铁硫碳纳米材料, 抗生素降解, 磺胺甲唑

Abstract:

Heterogeneous iron-based materials have been widely used in the degradation of organic pollutants by activating peroxymonosulfate (PMS) due to the significant effect and low cost,and how to effectively promote Fe²⁺/Fe³⁺ cycling in the catalysts and thus enhance the catalytic performance has always been the focus of research. Iron-sulfur doped carbon composites (Fe-SC) were prepared by a one-step calcination method using carrageenan as the natural S and C source. X-ray diffraction,scanning electron microscopy,and other characterization techniques were used to analyze the microscopic morphology and material composition of Fe-SC. Then it was applied to the activation of PMS for the degradation of sulfamethoxazole (SMX) to evaluate its catalytic performance. The results showed that the Fe-SC-900 had the best catalytic effect,and the Fe-SC-900/PMS could degrade 99.8% SMX at 40 min. In addition,the Fe-SC-900/PMS system was able to resist coexisting anions and natural organic matter,which had good potential for practical application. The degradation mechanism experiments showed the presence of ·OH, SO₄ ^·-, O₂ ^·- and ¹O₂ in the Fe-SC-900/PMS system,and ¹O₂and SO₄ ^·- had the major role in the SMX degradation.

Key words: advanced oxidation, peroxymonosulfate, iron-sulfur doped catalyst, antibiotics degradation, sulfamethoxazole

中图分类号:

X703.1

韦敏, 王榕, 刘士华, 佟宜霏. 铁硫掺杂碳纳米材料活化过硫酸盐降解磺胺甲唑[J]. 工业水处理, 2025, 45(8): 174-181.

Min WEI, Rong WANG, Shihua LIU, Yifei TONG. Degradation of sulfamethoxazole by activated peroxymonosulfate by iron sulfur doped carbon nanomaterials[J]. Industrial Water Treatment, 2025, 45(8): 174-181.

https://www.iwt.cn/CN/Y2025/V45/I8/174

图/表 13

图1 Fe-SC-x的XRD

Fig.1 XRD patterns of Fe-SC-x

图2 Fe-SC-900的SEM（a、b）和EDS-mapping（c、d）

Fig.2 SEM（a，b） and EDS-mapping（c，d） images of Fe-SC-900

图3 Fe-SC-900的XPS图谱

Fig.3 XPS spectrum of Fe-SC-900

图4 Fe-SC-x的催化性能

Fig.4 Catalytic properties of Fe-SC-x

图5 Fe-SC-900与已有报道的Fe/S掺杂碳纳米材料的k值比较

Fig.5 Comparison of reaction rate constants （k values） between Fe-SC-900 and previously reported Fe/S-doped carbon nanomaterials

图6 Fe-SC-900投加量对Fe-SC-900/PMS/SMX体系的影响

Fig.6 Influences of the dosage of Fe-SC-900 on the Fe-SC-900/PMS/SMX system

图7 PMS投加量对Fe-SC-900/PMS/SMX体系的影响

Fig.7 Influences of the dosage of PMS on the Fe-SC-900/PMS/SMX system

图8 初始pH对Fe-SC-900/PMS/SMX体系的影响

Fig.8 Influences of the initial pH on the Fe-SC-900/PMS/SMX system

图9 不同阴离子对Fe-SC-900/PMS/SMX体系的影响

Fig.9 Influences of different anions on the Fe-SC-900/PMS/SMX system

图10 HA对Fe-SC-900/PMS/SMX体系的影响

Fig. 10 Influences of HA on the Fe-SC-900/PMS/SMX system

图11 猝灭剂对Fe-SC-900/PMS/SMX体系的影响

Fig.11 Influences of quencher on the Fe-SC-900/PMS/SMX system

图12 Fe-SC-900/PMS体系中自由基的EPR

Fig.12 EPR spectra of reactive oxygen species in the Fe-SC-900/PMS system

图13 Fe-SC-900/PMS体系中铁循环验证

Fig.13 Effect of adding Fe³⁺ on Fe-SC-900/PMS system of SMX degradation

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