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