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新型 ZIF-67 衍生 Co@CNTs 纳米复合材料作为去除四环素和磺胺嘧啶抗生素的有效吸附剂。

Novel ZIF-67-derived Co@CNTs nanocomposites as effective adsorbents for removal of tetracycline and sulfadiazine antibiotics.

机构信息

School of Chemical and Energy Engineering, Faculty of Engineering, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor, Malaysia; Institute of Applied Technology and Sustainable Development, Nguyen Tat Thanh University, 298-300A Nguyen Tat Thanh, District 4, Ho Chi Minh City 755414, Viet Nam.

School of Chemical and Energy Engineering, Faculty of Engineering, Universiti Teknologi Malaysia, 81310 UTM Johor Bahru, Johor, Malaysia; Centre of Hydrogen Energy, Institute of Future Energy, 81310 UTM Johor Bahru, Johor, Malaysia.

出版信息

Environ Res. 2023 May 15;225:115516. doi: 10.1016/j.envres.2023.115516. Epub 2023 Feb 18.

Abstract

Tetracycline (TCC) and sulfadiazine (SDZ) are two of the most consumed antibiotics for human therapies and bacterial infection treatments in aquafarming fields, but their accumulative residues can result in negative effects on water and aquatic microorganisms. Removal techniques are therefore required to purify water before use. Herein, we concentrate on adsorptive removal of TCC and SDZ using cobalt@carbon nanotubes (Co@CNTs) derived from Co-ZIF-67. The presence of CNTs on the edge of nanocomposites was observed. Taguchi orthogonal array was designed with four variables including initial concentration (5-20 mg L), dosage (0.05-0.2 g L), time (60-240 min), and pH (2-10). Concentration and pH were found to be main contributors to adsorption of tetracycline and sulfadiazine, respectively. The optimum condition was found at concentration 5 mg L, dosage 0.2 g L, contact time 240 min, and pH 7 for both TCC and SDZ removals. Confirmation tests showed that Co@CNTs-700 removed 99.6% of TCC and 97.3% of SDZ with small errors (3-5.5%). Moreover, the kinetic and isotherm were studied, which kinetic and isotherm data were best fitted with pseudo second-order model and Langmuir. Maximum adsorption capacity values for TCC and SDZ were determined at 118.4-174.1 mg g for 180 min. We also proposed the main role of interactions such as hydrogen bonding, π-π stacking, and electrostatic attraction in the adsorption of antibiotics. With high adsorption performance, Co@CNTs-700 is expected to remove antibiotics efficiently from wastewater.

摘要

四环素 (TCC) 和磺胺嘧啶 (SDZ) 是水产养殖领域人类治疗和细菌感染治疗中使用最多的两种抗生素,但它们的累积残留会对水和水生微生物产生负面影响。因此,需要采用去除技术在使用前净化水。本文主要研究了利用 Co-ZIF-67 衍生的钴@碳纳米管 (Co@CNTs) 对 TCC 和 SDZ 进行吸附去除。观察到纳米复合材料边缘存在 CNTs。采用四变量(初始浓度(5-20 mg L)、剂量(0.05-0.2 g L)、时间(60-240 min)和 pH(2-10))的 Taguchi 正交数组设计。结果表明,浓度和 pH 分别是吸附四环素和磺胺嘧啶的主要影响因素。对于 TCC 和 SDZ 的去除,最佳条件为浓度 5 mg L、剂量 0.2 g L、接触时间 240 min 和 pH 7。验证试验表明,Co@CNTs-700 对 TCC 和 SDZ 的去除率分别达到 99.6%和 97.3%,误差较小(3-5.5%)。此外,还研究了动力学和等温线,动力学和等温线数据与拟二级模型和 Langmuir 拟合最好。TCC 和 SDZ 的最大吸附容量值在 180 min 时分别为 118.4-174.1 mg g。我们还提出了氢键、π-π堆积和静电吸引等相互作用在抗生素吸附中的主要作用。Co@CNTs-700 具有较高的吸附性能,有望从废水中高效去除抗生素。

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