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无定形氧化钴修饰的埃洛石纳米管用于过一硫酸盐激活的高效磺胺甲恶唑降解。

Amorphous cobalt oxide decorated halloysite nanotubes for efficient sulfamethoxazole degradation activated by peroxymonosulfate.

机构信息

School of Environmental Science and Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China; Institute for Ecological Research and Pollution Control of Plateau Lakes, Institute of International Rivers and Eco-Security, School of Ecology and Environmental Science, Yunnan University, Kunming 650504, China.

School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252000, China.

出版信息

J Colloid Interface Sci. 2022 Feb;607(Pt 1):857-868. doi: 10.1016/j.jcis.2021.08.168. Epub 2021 Sep 9.

Abstract

In this study, a new hollow nanotube material, 30% Co-CHNTs was prepared by the impregnation-chemical reduction-calcination method. This material can be used as a peroxymonosulfate (PMS) activator to catalyse the degradation of sulfamethoxazole (SMX). The best reaction conditions that correspond to the degradation rate of SMX, up to 97.5%, are as follows: the concentration of SMX is 10 mg L, the amount of catalyst is 0.20 g L, the dosage is 1.625 mM, and the solution pH is 6.00. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma optical emission spectrometry (ICP-OES) show that the calcined composites mainly stimulate an increase in the content of bivalent cobalt in PMS and reduce the leaching of cobalt ions after the reaction. Additionally, the 30% Co-CHNTs + PMS reaction system exhibits a reasonable SMX degradation rate in a natural organic matter solution and excellent stability after three repeated experiments. Furthermore, the possible degradation mechanism in the 30% Co-CHNTs + PMS reaction system was analysed through electron paramagnetic resonance (EPR) and free-radical capture experiments, and it was observed that the non-radical degradation of O plays a leading role in SMX degradation. Finally, according to the nine degradation intermediates detected by liquid chromatography-mass spectrometry (LC-MS), four possible SMX degradation routes were proposed. This study proved that a 30% Co-CHNTs heterogeneous catalyst is easily prepared, inexpensive, and environmentally friendly and has potential application in antibiotic wastewater treatment.

摘要

在这项研究中,通过浸渍-化学还原-煅烧法制备了一种新型的中空纳米管材料,30%Co-CHNTs。该材料可用作过一硫酸盐(PMS)的活化剂来催化降解磺胺甲恶唑(SMX)。对应 SMX 降解率高达 97.5%的最佳反应条件如下:SMX 浓度为 10mg L、催化剂用量为 0.20g L、剂量为 1.625mM 和溶液 pH 值为 6.00。X 射线光电子能谱(XPS)和电感耦合等离子体发射光谱(ICP-OES)表明,煅烧后的复合材料主要刺激 PMS 中二价钴含量的增加,并减少了反应后钴离子的浸出。此外,30%Co-CHNTs+PMS 反应体系在天然有机物溶液中具有合理的 SMX 降解速率和三次重复实验后的良好稳定性。此外,通过电子顺磁共振(EPR)和自由基捕获实验分析了 30%Co-CHNTs+PMS 反应体系中的可能降解机制,观察到非自由基降解 O 在 SMX 降解中起主导作用。最后,根据液相色谱-质谱(LC-MS)检测到的 9 个降解中间产物,提出了 4 种可能的 SMX 降解途径。这项研究证明了 30%Co-CHNTs 多相催化剂易于制备、成本低、环保,在抗生素废水处理方面具有潜在应用。

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