Liu Longjie, Xu Qianyu, Owens Gary, Chen Zuliang
School of Environmental Science and Engineering, Fujian Normal University, Fuzhou, 350007, Fujian Province, China.
Environmental Contaminants Group, Future Industries Institute, University of South Australia, Mawson Lakes, SA, 5095, Australia.
J Hazard Mater. 2021 Jan 15;402:123544. doi: 10.1016/j.jhazmat.2020.123544. Epub 2020 Jul 25.
Antibiotics are an emerging class of persistent contaminants that are now of major environmental concern because they pose potential risks to both environmental and human health. Here reduced graphene oxide composited with bimetallic iron/palladium nanoparticles (rGO@nFe/Pd) was synthesized via a green tea extract and used to remove a common antibiotic, rifampicin from aqueous solution. The innate physical rifampicin removal efficiency of the composite (79.9 %) was increased to 85.7 % when combined with Fenton-oxidation. The mechanism and the main factors controlling Fenton-oxidation of rifampicin by rGO@nFe/Pd were investigated. Oxidation followed a pseudo-second-order degradation kinetic model with an activation energy of 47.3 kJ mol. rGO@nFe/Pd were characterized by Brunauer-Emmett-Teller (BET), fourier transform infrared (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray energy spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), X-Ray powder diffraction (XRD), and zeta potential. Rifampicin degradation products observed by LC-UV, where subsequently confirmed to be mainly 5,6,9-trihydroxynaphtho [2,1-b] furan-1(2 H)-one, 5,6-dihydroxy-1-oxo-1,2-dihydronaphtho [2,1-b] furan-2-yl formate and (S)-5,6,9-trihydroxy-2-(3-methoxypropoxy)-2-methylnaphtho [2,1-b] furan-1(2 H)-one by LC-MS. Finally, the practical effectiveness of the composite material for antibiotic removal was demonstrated by the treatment of representative wastewaters, where rifampicin removal efficiencies of 80.4, 77.9 and 70.2 % were observed for river, aquaculture wastewater and domestic wastewater, respectively.
抗生素是一类新出现的持久性污染物,由于它们对环境和人类健康都构成潜在风险,目前已成为主要的环境问题。本文通过绿茶提取物合成了还原氧化石墨烯复合双金属铁/钯纳米颗粒(rGO@nFe/Pd),并用于从水溶液中去除一种常见抗生素利福平。该复合材料对利福平的固有物理去除效率(79.9%)在与芬顿氧化结合时提高到了85.7%。研究了rGO@nFe/Pd对利福平进行芬顿氧化的机理及主要控制因素。氧化过程遵循准二级降解动力学模型,活化能为47.3 kJ/mol。通过布鲁诺尔-埃米特-特勒(BET)、傅里叶变换红外光谱(FTIR)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线能谱(EDS)、X射线光电子能谱(XPS)、X射线粉末衍射(XRD)和zeta电位对rGO@nFe/Pd进行了表征。通过液相色谱-紫外检测观察到利福平降解产物,随后通过液相色谱-质谱确认为主要为5,6,9-三羟基萘并[2,1-b]呋喃-1(2H)-酮、5,6-二羟基-1-氧代-1,2-二氢萘并[2,1-b]呋喃-2-基甲酸酯和(S)-5,6,9-三羟基-2-(3-甲氧基丙氧基)-2-甲基萘并[2,1-b]呋喃-1(2H)-酮。最后,通过处理典型废水证明了该复合材料去除抗生素的实际效果,其中河水、水产养殖废水和生活污水中利福平的去除效率分别为80.4%、77.9%和70.2%。