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负载碳纳米管的铜镍铁氧体活化过硫酸盐体系用于吸附和降解盐酸土霉素

Carbon nanotube-loaded copper-nickel ferrite activated persulfate system for adsorption and degradation of oxytetracycline hydrochloride.

作者信息

Ma Yuting, Wang Rong, Gao Chenping, Han Runping

机构信息

College of Chemistry, Zhengzhou University, No 100 of Kexue Road, Zhengzhou 450001, China.

College of Chemistry, Zhengzhou University, No 100 of Kexue Road, Zhengzhou 450001, China.

出版信息

J Colloid Interface Sci. 2023 Jun 15;640:761-774. doi: 10.1016/j.jcis.2023.03.001. Epub 2023 Mar 4.

Abstract

In this study, a new composite (MWCNTs-CuNiFeO) prepared by loading magnetic CuNiFeO particles onto carboxylated carbon nanotubes (MWCNTs) through co-precipitation was applied to remove oxytetracycline hydrochloride (OTC-HCl) in solution. The magnetic properties of this composite could address of the issue of difficulty associated with the separation of MWCNTs from mixtures when applied as an adsorbent. In addition to the good adsorption properties recorded for MWCNTs-CuNiFeO towards OTC-HCl, this developed composite could be used to activate potassium persulfate (KPS) for an efficient degradation of OTC-HCl. The MWCNTs-CuNiFeO was systematically characterized using Vibrating Sample Magnetometer (VSM), Electron Paramagnetic Resonance (EPR) and X-ray Photoelectron Spectroscopy (XPS). The influence of dose of MWCNTs-CuNiFeO, the initial pH, the amount of KPS and the reaction temperature on the adsorption and degradation of OTC-HCl by MWCNTs-CuNiFeO were discussed. The adsorption and degradation experiments showed that MWCNTs-CuNiFeO exhibited an adsorption capacity of 270 mg·g for OTC-HCl with the removal efficiency 88.6% at 303 K (at an initial pH 3.52, 5 mg KPS, 10 mg composite, 10 mL reaction concentration 300 mg·L of OTC-HCl). The Langmuir and Koble-Corrigan models were used to describe the equilibrium process while the Elovich equation and Double constant model were suitable to describe the kinetic process. The adsorption process was based on single-molecule layer reaction and non-homogeneous diffusion process. The mechanisms of adsorption were complexation and hydrogen bond whereas active species such as SO, OH and O were confirmed to have played a major role in the degradation of OTC-HCl. The composite was also found to be very stable with good reusability property. These results confirm the good potential associated with the use of MWCNTs-CuNiFeO/KPS system for the removal of some typical pollutants from wastewater.

摘要

在本研究中,通过共沉淀法将磁性CuNiFeO颗粒负载到羧基化碳纳米管(MWCNTs)上制备的新型复合材料(MWCNTs-CuNiFeO)被用于去除溶液中的盐酸土霉素(OTC-HCl)。该复合材料的磁性能够解决MWCNTs作为吸附剂应用时从混合物中分离困难的问题。除了MWCNTs-CuNiFeO对OTC-HCl具有良好的吸附性能外,这种开发的复合材料还可用于活化过硫酸钾(KPS)以有效降解OTC-HCl。使用振动样品磁强计(VSM)、电子顺磁共振(EPR)和X射线光电子能谱(XPS)对MWCNTs-CuNiFeO进行了系统表征。讨论了MWCNTs-CuNiFeO的用量、初始pH值、KPS用量和反应温度对MWCNTs-CuNiFeO吸附和降解OTC-HCl的影响。吸附和降解实验表明,MWCNTs-CuNiFeO在303K时对OTC-HCl的吸附容量为270mg·g,去除效率为88.6%(初始pH值为3.52,5mg KPS,10mg复合材料,10mL反应浓度为300mg·L的OTC-HCl)。采用Langmuir和Koble-Corrigan模型描述平衡过程,而Elovich方程和双常数模型适用于描述动力学过程。吸附过程基于单分子层反应和非均相扩散过程。吸附机制为络合和氢键作用,而SO、OH和O等活性物种被证实对OTC-HCl的降解起主要作用。还发现该复合材料非常稳定,具有良好的可重复使用性。这些结果证实了使用MWCNTs-CuNiFeO/KPS系统从废水中去除一些典型污染物具有良好的潜力。

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