过渡金属硒化物上的双金属氧化还原驱动 PMS 快速活化以降解磺胺甲噁唑:机理、降解途径和中间体毒性

IF 2.8 4区 生物学 Q3 BIOTECHNOLOGY & APPLIED MICROBIOLOGY Journal of chemical technology and biotechnology Pub Date : 2024-09-06 DOI:10.1002/jctb.7748
Yongming Wang, Qiang Chen, Yuezong Su, Yuxuan He, Jin Qian, Kailin Xu
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引用次数: 0

摘要

背景抗生素在水生环境中的存在日益增加,对生态环境造成了巨大的风险,磺胺甲噁唑(SMX)就是一个突出的例子,因为它具有持久性,而且在医疗和兽医实践中被广泛使用。高级氧化工艺,尤其是基于过氧单硫酸盐(PMS)的氧化工艺,在降解此类污染物方面已显示出良好的前景。结果在催化剂用量为 0.25 克/升、PMS 用量为 1.5 克/升的情况下,SMX 降解率超过 95%,这表明 FM 是一种有效的 PMS 激活剂,能够高效氧化 SMX。EPR 测试和淬灭实验证实降解体系中存在 1O2、SO4-- 和 -OH,其中 SO4--占主导地位。钼与铁的氧化还原循环参与了 PMS 的活化。此外,SMX 分子的 DFT 计算显示,易损位点主要在磺酰胺基团和含氧基团附近。毒性评估显示,SMX 的大部分初级降解中间产物都具有毒性,而进一步的小分子产物则无毒。最终降解产物的低毒性进一步证明了这种方法的环境安全性,使其成为现实世界中水处理应用的理想候选方案。© 2024 化学工业学会(SCI)。
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Rapid activation of PMS driven by bimetallic redox on transition metal selenides for sulfamethoxazole degradation: mechanism, degradation pathway and intermediates toxicity

BACKGROUND

The increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe2/MoSe2 (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX.

RESULTS

Over 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of 1O2, SO4•– and OH in the degradation system, with SO4•- predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen-containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non-toxic.

CONCLUSION

This work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real-world water treatment applications. © 2024 Society of Chemical Industry (SCI).

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来源期刊
CiteScore
7.00
自引率
5.90%
发文量
268
审稿时长
1.7 months
期刊介绍: Journal of Chemical Technology and Biotechnology(JCTB) is an international, inter-disciplinary peer-reviewed journal concerned with the application of scientific discoveries and advancements in chemical and biological technology that aim towards economically and environmentally sustainable industrial processes.
期刊最新文献
Issue Information In Focus: Materials and the Environment Symposium (XXXI IMRC México) Issue Information Adsorption behavior of graphite‐like walnut shell biochar modified with ammonia for ciprofloxacin in aqueous solution Eco‐friendly approaches for synthesis of indolyl 1H‐pyrroles using rice‐husk‐derived carbonaceous sulfonation as the green catalyst
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