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一锅法制备污泥衍生的磁性 Fe、N 共掺杂碳催化剂用于过一硫酸盐诱导消除酚类污染物。

One-pot fabrication of sludge-derived magnetic Fe,N-codoped carbon catalysts for peroxymonosulfate-induced elimination of phenolic contaminants.

机构信息

Institute of Chemistry, Henan Academy of Sciences, Zhengzhou, 450002, PR China.

Institute of Chemistry, Henan Academy of Sciences, Zhengzhou, 450002, PR China.

出版信息

Chemosphere. 2020 Jun;248:126076. doi: 10.1016/j.chemosphere.2020.126076. Epub 2020 Jan 31.

Abstract

The use of waste sludge as a precursor of catalysts for environmental applications has been encouraged during the past few years. In this study, a series of magnetic Fe,N-codoped carbon catalysts (UBC-x) were successfully prepared by a facile one-pot pyrolysis method using Fe-rich sludge and N-rich urea as the raw materials. By carefully controlling the mass ratio of urea/dry sludge (x = 0-3), a significant amount of N (1-10 mass%) were incorporated, and the UBC-x catalysts, especially UBC-0.5 and UBC-0.75, could be imparted with high catalytic activity, convenient magnetic separation and high recycle stability. Phenolic contaminants like phenol and bisphenol A (BPA) could be nearly completely removed through peroxymonosulfate (PMS)-induced degradation by using UBC-x as the catalysts under a wide pH range (2-11) and with the co-existence of water constituents (chloride Cl and sodium humate NaH, 0-50 mM). Among the several reactive oxidative species (ROS), singlet oxygen (O) was deemed as the main reactive species responsible for BPA degradation. Both Fe and N active sites contributed to the high catalytic activity of UBC-x, and their coordination made the catalysts rather stable with no significant Fe leaching under a wide pH range. Therefore, after an easy magnetic separation, the UBC-x could be recycled and reused efficiently in another BPA removal cycle. The as-synthesized magnetic Fe,N-codoped carbon catalysts provided a new route for sludge reutilization and showed potential applications in wastewater treatment.

摘要

在过去的几年中,人们鼓励将废污泥用作环境应用催化剂的前体。在这项研究中,通过简便的一锅热解法成功制备了一系列磁性 Fe,N 共掺杂碳催化剂(UBC-x),该方法使用富铁污泥和富氮尿素作为原料。通过仔细控制尿素/干污泥的质量比(x=0-3),可以掺入大量的 N(1-10 质量%),并且 UBC-x 催化剂,尤其是 UBC-0.5 和 UBC-0.75,可以具有高催化活性、方便的磁性分离和高循环稳定性。通过使用 UBC-x 作为催化剂,在很宽的 pH 范围(2-11)和共存水成分(氯离子 Cl 和腐植酸钠 NaH,0-50 mM)下,过一硫酸盐(PMS)诱导降解可以几乎完全去除酚类污染物,如苯酚和双酚 A(BPA)。在几种活性氧化物种(ROS)中,单线态氧(O)被认为是导致 BPA 降解的主要活性物种。Fe 和 N 活性位点都有助于 UBC-x 的高催化活性,它们的配位使催化剂在很宽的 pH 范围内相当稳定,没有明显的 Fe 浸出。因此,在进行简单的磁性分离后,UBC-x 可以在另一个 BPA 去除循环中有效回收和再利用。合成的磁性 Fe,N 共掺杂碳催化剂为污泥再利用提供了一条新途径,并显示出在废水处理中的潜在应用。

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