Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University , Wuhan 430079, P. R. China.
Environ Sci Technol. 2017 May 2;51(9):5118-5126. doi: 10.1021/acs.est.6b05906. Epub 2017 Apr 11.
In this study, we construct a surface Fenton system with hydroxylamine (NHOH), goethite (α-FeOOH), and HO (α-FeOOH-HA/HO) to degrade various organic pollutants including dyes (methyl orange, methylene blue, and rhodamine B), pesticides (pentachlorophenol, alachlor, and atrazine), and antibiotics (tetracycline, chloramphenicol, and lincomycin) at pH 5.0. In this surface Fenton system, the presence of NHOH could greatly promote the HO decomposition on the α-FeOOH surface to produce ·OH without releasing any detectable iron ions during the alachlor degradation, which was different from some previously reported heterogeneous Fenton counterparts. Moreover, the ·OH generation rate constant of this surface Fenton system was 10-10 times those of previous heterogeneous Fenton processes. The interaction between α-FeOOH and NHOH was investigated with using attenuated total reflectance Fourier transform infrared spectroscopy and density functional theory calculations. The effective degradation of organic pollutants in this surface Fenton system was ascribed to the efficient Fe(III)/Fe(II) cycle on the α-FeOOH surface promoted by NHOH, which was confirmed by X-ray photoelectron spectroscopy analysis. The degradation intermediates and mineralization of alachlor in this surface Fenton system were then systematically investigated using total organic carbon and ion chromatography, liquid chromatography-mass spectrometry, and gas chromatography-mass spectrometry. This study offers a new strategy to degrade organic pollutants and also sheds light on the environmental effects of goethite.
在这项研究中,我们构建了一个表面芬顿系统,使用羟胺(NHOH)、针铁矿(α-FeOOH)和 HO(α-FeOOH-HA/HO)来降解各种有机污染物,包括染料(甲基橙、亚甲基蓝和罗丹明 B)、农药(五氯苯酚、莠去津和阿特拉津)和抗生素(四环素、氯霉素和林可霉素),pH 值为 5.0。在这个表面芬顿系统中,NHOH 的存在可以极大地促进 HO 在α-FeOOH 表面的分解,产生·OH,而在莠去津降解过程中没有释放任何可检测到的铁离子,这与一些以前报道的非均相芬顿类似物不同。此外,这个表面芬顿系统的·OH 生成速率常数是以前的非均相芬顿过程的 10-10 倍。通过衰减全反射傅里叶变换红外光谱和密度泛函理论计算研究了α-FeOOH 和 NHOH 之间的相互作用。有机污染物在这个表面芬顿系统中的有效降解归因于 NHOH 促进的α-FeOOH 表面上的有效 Fe(III)/Fe(II)循环,这通过 X 射线光电子能谱分析得到了证实。然后,使用总有机碳和离子色谱、液相色谱-质谱、气相色谱-质谱系统地研究了这个表面芬顿系统中莠去津的降解中间体和矿化作用。这项研究提供了一种降解有机污染物的新策略,也为针铁矿的环境效应提供了新的思路。