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在弱碱性条件下使用 Co-SAM-SCS/HO Fenton 类系统高效降解模拟和实际废水中的磺胺甲恶唑。

Efficient degradation of sulfamethazine in simulated and real wastewater at slightly basic pH values using Co-SAM-SCS /HO Fenton-like system.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.

College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.

出版信息

Water Res. 2018 Jul 1;138:7-18. doi: 10.1016/j.watres.2018.03.022. Epub 2018 Mar 10.

Abstract

The presence of antibiotics in aquatic environments has attracted global concern. Fenton process is an attractive yet challenging method for antibiotics degradation, especially when such a reaction can be conducted at neutral pH values. In this study, a novel composite Fe/Co catalyst was synthesized via the modification of steel converter slag (SCS) by salicylic acid-methanol (SAM) and cobalt nitrate (Co(NO)). The catalysts were characterized by N-Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), Fourier transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). The results indicated that the Co-SAM-SCS/HO Fenton-like system was very effective for sulfamethazine (SMZ) degradation at a wide pH range. At initial pH of 7.0, the degradation rate of SMZ in Co-SAM-SCS/HO system was 2.48, 3.20, 6.18, and 16.21 times of that in Fe-SAM-SCS/HO, SAM-SCS/HO, Co(NO)/HO and SCS/HO system, respectively. The preliminary analysis suggested that high surface area of Co-SAM-SCS sample and synergistic effect between introduced Co and SAM-SCS are responsible for the efficient catalytic activity. During the degradation, three main intermediates were identified by high performance liquid chromatography-mass spectrometry (HPLC-MS) analysis. Based on this, a possible degradation pathway was proposed. The SEM images, XRD patterns and XPS spectra before and after the reactions demonstrate that the crystal and chemical structure of Co-SAM-SCS after five cycles are almost unchanged. Besides, the Co-SAM-SCS presented low iron and cobalt leaching (0.17 mg/L and 2.36 mg/L, respectively). The studied Fenton-like process also showed high degradation of SMZ in river water and municipal wastewater. The progress will bring valuable insights to develop high-performance heterogeneous Fenton-like catalysts for environmental remediation.

摘要

抗生素在水环境中的存在引起了全球关注。芬顿工艺是一种有吸引力但具有挑战性的抗生素降解方法,特别是当这种反应可以在中性 pH 值下进行时。在这项研究中,通过水杨酸-甲醇(SAM)和硝酸钴(Co(NO))对炼钢转炉渣(SCS)进行修饰,合成了一种新型复合 Fe/Co 催化剂。通过 N2- Brunauer-Emmett-Teller(BET)、X 射线衍射(XRD)、傅里叶变换红外(FT-IR)、X 射线光电子能谱(XPS)、扫描电子显微镜(SEM)和能谱(EDS)对催化剂进行了表征。结果表明,Co-SAM-SCS/HO 类芬顿体系在很宽的 pH 范围内对磺胺甲恶唑(SMZ)的降解非常有效。在初始 pH 为 7.0 时,Co-SAM-SCS/HO 体系中 SMZ 的降解速率分别是 Fe-SAM-SCS/HO、SAM-SCS/HO、Co(NO)/HO 和 SCS/HO 体系的 2.48、3.20、6.18 和 16.21 倍。初步分析表明,Co-SAM-SCS 样品的高表面积和引入的 Co 与 SAM-SCS 之间的协同效应是其高效催化活性的原因。在降解过程中,通过高效液相色谱-质谱(HPLC-MS)分析鉴定了三种主要的中间产物。在此基础上,提出了可能的降解途径。反应前后的 SEM 图像、XRD 图谱和 XPS 谱表明,反应后 Co-SAM-SCS 的晶体和化学结构几乎没有变化。此外,Co-SAM-SCS 的铁和钴浸出率较低(分别为 0.17 mg/L 和 2.36 mg/L)。所研究的类芬顿工艺在河水和城市废水中也表现出了对 SMZ 的高效降解。该研究进展将为开发用于环境修复的高性能非均相类芬顿催化剂提供有价值的见解。

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