Controllable synthesis of mesoporous manganese oxide microsphere efficient for photo-Fenton-like removal of fluoroquinolone antibiotics
Controllable synthesis of mesoporous manganese oxide microsphere efficient for photo-Fenton-like removal of fluoroquinolone antibiotics
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介孔氧化锰微球的可控合成可有效光芬顿去除氟喹诺酮类抗生素
DOI：
10.1016/j.apcatb.2019.02.034
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发表时间：
2019-07-05
影响因子：
22.1
通讯作者：
Yan, Kai
中科院分区：
文献类型：
--
作者：
Wang, Anqi;Wang, Hui;Yan, Kai
采用软模板剂P123辅助法成功地实现了介孔锰氧化物微球的可控合成。所获得的MnOx材料对于去除氟喹诺酮类抗生素（即，氧氟沙星、环丙沙星、恩诺沙星和左氧氟沙星），使用过氧单硫酸盐（PMS）作为氧化剂，在UV或模拟阳光照射下。在2 g P123（P-2-Mn 3 O 4）存在下制备的介孔Mn 3 O 4微球对氟喹诺酮类抗生素具有上级催化活性，在紫外光照射下10 min内几乎完全降解。在模拟太阳光照射下，P-2-Mn 3 O 4对氧氟沙星、环丙沙星、恩诺沙星和左氧氟沙星的降解率分别为74.5%、79.4%、72.3%和81.9%，且催化剂在连续多次运行后仍保持稳定，催化活性未发生明显失活，结构未发生明显变化，并且观察到Mn离子的轻微浸出。ESR谱进一步证实了SO 4中心点、（OH）-O中心点、O-2（中心点-）和O-1（2）自由基在抗生素分子的分解过程中起着重要作用。最后，对反应动力学进行了研究，并提出了合理的降解途径.
Controllable synthesis of mesoporous manganese oxide (MnOx) microsphere is successfully achieved using a soft-template P123 assisted method. The as-obtained MnOx materials are highly efficient and versatile to remove the category of fluoroquinolone antibiotics (i.e., ofloxacin, ciprofloxacin, enrofloxacin and levofloxacin) using peroxymonosulfate (PMS) as the oxidant under UV or simulated sunlight irradiation. The mesoporous Mn3O4 microsphere prepared in the presence of 2 g P123 (P-2-Mn3O4) exhibits the superior catalytic activity with almost perfect degradation for the fluoroquinolone antibiotics in 10 min under UV irradiation. Moreover, under simulated sunlight irradiation, 74.5% of ofloxacin, 79.4% of ciprofloxacin, 72.3% of enrofloxacin and 81.9% of levofloxacin can be degraded by P-2-Mn3O4 in 10 min. Besides, the P-2-Mn(3)O(4)catalyst maintains stable without the obvious deactivation of catalytic activity or structural change after several successive runs, and slight leaching of Mn ions is observed. The ESR spectra further document that SO4 center dot-, (OH)-O-center dot, O-2(center dot-) and O-1(2) radicals are prominent in the decomposition process of antibiotic molecules. In the end, the reaction kinetic and rational degradation pathway are also investigated and proposed.