School of Resources and Environment, Anhui Agricultural University, Hefei 230036, China.
Key Laboratory for Agri-Food Safety, Anhui Agricultural University, Hefei 230036, China.
Int J Environ Res Public Health. 2019 Jun 27;16(13):2270. doi: 10.3390/ijerph16132270.
The removal of tetracycline antibiotics from water is currently an important environmental issue. Here we prepared an iron-loaded granular activated carbon catalyst (GAC-Fe) through a one-step calcination method to remove tetracycline antibiotics from aqueous solution. The GAC-Fe was characterized by Fourier transform infrared absorption spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction analysis. The effect of different influencing factors on the removal behavior of tetracycline antibiotics was studied, such as the solid-to-liquid ratio, HO dosage, environmental temperature, initial pH, and contact time. The removal mechanism was explored through Fe ion dissolution and a free radical quenching experiment. The results show that the optimum solid-to-liquid ratio was 3.0 g∙L and the suitable HO dosage was 1.0 mL (3%). The applicable environmental temperature was 25 °C and the appropriate pH value was 2.0. The removal rate of tetracycline antibiotics tended to be stable in a contact time of 600 min. The main mechanism of tetracycline antibiotic removal by GAC-Fe was heterogeneous catalytic reaction through iron ion leaching and free radical inhibition experiment. The hydroxyl radical played a major role during the removal process. The partially dissolved iron ions initiated a homogeneous catalytic reaction. However, heterogeneous catalytic degradation was the main reaction. The GAC-Fe could still remove tetracycline antibiotics after five cycles, especially for methacycline and minocycline. Our work suggests that the GAC-Fe catalyst has potential as a remediation agent for tetracycline antibiotics in aqueous solution.
从水中去除四环素类抗生素目前是一个重要的环境问题。在这里,我们通过一步煅烧法制备了负载铁的颗粒活性炭催化剂(GAC-Fe),用于从水溶液中去除四环素类抗生素。通过傅里叶变换红外吸收光谱、X 射线光电子能谱和 X 射线衍射分析对 GAC-Fe 进行了表征。研究了不同影响因素对四环素类抗生素去除行为的影响,如固液比、HO 用量、环境温度、初始 pH 值和接触时间。通过 Fe 离子溶解和自由基淬灭实验探讨了去除机制。结果表明,最佳固液比为 3.0 g·L,适宜的 HO 用量为 1.0 mL(3%)。适用的环境温度为 25°C,合适的 pH 值为 2.0。在 600 min 的接触时间内,四环素类抗生素的去除率趋于稳定。GAC-Fe 去除四环素类抗生素的主要机制是通过铁离子浸出和自由基抑制实验进行的非均相催化反应。羟基自由基在去除过程中起主要作用。部分溶解的铁离子引发均相催化反应。然而,非均相催化降解是主要反应。GAC-Fe 在经过五次循环后仍能去除四环素类抗生素,特别是甲烯土霉素和米诺环素。我们的工作表明,GAC-Fe 催化剂作为水溶液中四环素类抗生素的修复剂具有潜力。