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单原子铁固定在氮掺杂多孔碳上增强芬顿-like 降解磺胺嘧啶。

Enhanced Fenton-like degradation of sulfadiazine by single atom iron materials fixed on nitrogen-doped porous carbon.

机构信息

Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, PR China; Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China.

Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, PR China; Department of Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, PR China.

出版信息

J Colloid Interface Sci. 2021 Sep;597:56-65. doi: 10.1016/j.jcis.2021.03.168. Epub 2021 Apr 1.

Abstract

The use of single-atom iron catalysts in heterogeneous Fenton-like reactions has demonstrated tremendous potential for antibiotic wastewater treatment. In this study, single-atom iron fixed on nitrogen-doped porous carbon materials (Fe-ISAs@CN) was synthesised using a metal organic framework (MOF) as a precursor. Fe-ISAs@CN was applied as a heterogeneous Fenton catalyst to activate HO for the degradation of sulfadiazine (SDZ) in an aqueous solution. The physical and chemical properties of Fe-ISAs@CN were characterised by scanning electron microscopy (SEM), transmission electron microscope (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and rotating disk electrode (RDE) measurements. The results of our degradation experiments indicated that Fe-ISAs@CN exhibited remarkable activity and stability for the degradation of SDZ over a wide pH range; even after five cycles, Fe-ISAs@CN retained a high catalytic efficiency (>80%). The 5,5-dimethyl-1-oxaporphyrin-n-oxide (DMPO)-X signal captured by electron paramagnetic resonance (EPR) spectroscopy indicated that a large amount of hydroxyl radicals (OH) was produced in the reaction system. Quench tests indicated that the OH was the main active substance in the degradation of SDZ. The degradation products of the reaction were analysed by High Performance Liquid Chromatography-Mass Spectrometry (HPLC-MS), and possible degradation pathways for the SDZ degradation were proposed.

摘要

单原子铁催化剂在非均相类芬顿反应中的应用在抗生素废水处理方面展现出了巨大的潜力。在本研究中,使用金属有机骨架(MOF)作为前体制备了负载在氮掺杂多孔碳材料上的单原子铁(Fe-ISAs@CN)。将 Fe-ISAs@CN 用作非均相类芬顿催化剂,以 HO 激活剂的形式在水溶液中降解磺胺嘧啶(SDZ)。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、高角度环形暗场扫描透射电子显微镜(HAADF-STEM)、X 射线衍射(XRD)、X 射线光电子能谱(XPS)和旋转圆盘电极(RDE)测量对 Fe-ISAs@CN 的物理化学性质进行了表征。降解实验的结果表明,Fe-ISAs@CN 在很宽的 pH 范围内对 SDZ 的降解表现出显著的活性和稳定性;即使经过五次循环,Fe-ISAs@CN 仍保持着较高的催化效率(>80%)。电子顺磁共振(EPR)光谱捕捉到的 5,5-二甲基-1-氧杂卟啉-n-氧化物(DMPO)-X 信号表明,反应体系中产生了大量的羟基自由基(OH)。猝灭实验表明,OH 是 SDZ 降解的主要活性物质。通过高效液相色谱-质谱联用(HPLC-MS)对反应的降解产物进行了分析,并提出了可能的 SDZ 降解途径。

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