Aaron Albert Aryee , Alam Venugopal Narendra Kumar , Won Sik Shin
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The pseudo-second-order kinetic model and Langmuir model were used to described the uptake and equilibrium process in DCF/PA@Hem<sub>700</sub> system. Scavenging and electron-spin-resonance studies showed a non-radical singlet oxygen species (<sup>1</sup>O<sub>2</sub>) dominates over <sup>•</sup>OH and SO<sub>4</sub><sup>•−</sup> radicals in the system. The role of electron transfer was also verified via chronoamperometry and electrochemical-impedance spectroscopy techniques. Furthermore, the PA@Hem<sub>700</sub>/PMS remained highly active towards DCF degradation even in the presence of common anions, humic acid, and various water matrices. The developed catalyst exhibited a TOC removal of 65.8 %. The study also established the potential of PA@Hem<sub>700</sub>/PMS to degrade other organic pollutants (e.g., tetracycline (TC), simazine (SIM), and sulfamethoxazole (SMX)). 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引用次数: 0
摘要
本研究以血红素(Hem)和聚丙烯酸酯(PA)为原料,通过一步热解的方式合成了Fe参与的n掺杂碳催化剂PA@Hemx (x =热解温度)。所报道的方法使铁和N活性位点在PA衍生碳上的高分散和暴露成为可能。PA@Hemx样品随后用于过氧单硫酸盐(PMS)活化双氯芬酸(DCF)降解。表征研究的结果证实了血红素在复合材料中的成功结合。在pH = 6.01时,使用0.1 g L−1 PA@Hem700和1.0 mM PMS,在60分钟内实现了约99.2%的DCF降解。采用拟二级动力学模型和Langmuir模型描述了DCF/PA@Hem700体系的吸收和平衡过程。清除和电子自旋共振研究表明,非自由基单线态氧(1O2)在体系中占主导地位,而不是•OH和SO4•−自由基。电子转移的作用也通过计时电流法和电化学阻抗谱技术得到验证。此外,PA@Hem700/PMS即使在普通阴离子、腐植酸和各种水基质存在的情况下,对DCF的降解也保持高度活性。该催化剂的TOC去除率为65.8%。该研究还确定了PA@Hem700/PMS降解其他有机污染物(如四环素(TC),辛(SIM)和磺胺甲恶唑(SMX))的潜力。该研究结果有望推动其他新型聚合物基Fe/ N-C催化剂的合成研究,用于降解有机污染物。
Novel hemin-derived Fe/N–C magnetic catalyst for enhanced peroxymonosulfate activation and diclofenac degradation
In this study, Fe involved N-doped carbon catalysts labelled as PA@Hemx (x = pyrolysis temperature) was synthesized through a one-step pyrolysis of hemin (Hem) and polyacrylate (PA). The reported method enables high dispersion and exposure of both Fe and N active sites on PA derived carbon. The PA@Hemx samples were then used for peroxymonosulfate (PMS) activated diclofenac (DCF) degradation. Results from the characterization studies verified the successful incorporation of hemin in the composite. Approximately 99.2 % DCF degradation at pH = 6.01 was achieved in 60 min using 0.1 g L−1 PA@Hem700 and 1.0 mM PMS. The pseudo-second-order kinetic model and Langmuir model were used to described the uptake and equilibrium process in DCF/PA@Hem700 system. Scavenging and electron-spin-resonance studies showed a non-radical singlet oxygen species (1O2) dominates over •OH and SO4•− radicals in the system. The role of electron transfer was also verified via chronoamperometry and electrochemical-impedance spectroscopy techniques. Furthermore, the PA@Hem700/PMS remained highly active towards DCF degradation even in the presence of common anions, humic acid, and various water matrices. The developed catalyst exhibited a TOC removal of 65.8 %. The study also established the potential of PA@Hem700/PMS to degrade other organic pollutants (e.g., tetracycline (TC), simazine (SIM), and sulfamethoxazole (SMX)). The results from this study are expected to advance research on synthesizing other novel polymer-based Fe/N–C catalysts for degrading organic pollutants.
期刊介绍:
Chemosphere, being an international multidisciplinary journal, is dedicated to publishing original communications and review articles on chemicals in the environment. The scope covers a wide range of topics, including the identification, quantification, behavior, fate, toxicology, treatment, and remediation of chemicals in the bio-, hydro-, litho-, and atmosphere, ensuring the broad dissemination of research in this field.