Enhanced thermal activation of peroxymonosulfate by activated carbon for efficient removal of perfluorooctanoic acid

被引:87
作者
Liu, Guanhong [1 ]
Li, Chao [1 ]
Stewart, Brittney Ashley [1 ]
Liu, Lin [1 ]
Zhang, Meng [1 ]
Yang, Mingyang [2 ]
Lin, Kuangfei [1 ]
机构
[1] East China Univ Sci & Technol, State Environm Protect Key Lab Environm Risk Asse, Sch Resource & Environm Engn, Shanghai 200237, Peoples R China
[2] Delft Univ Technol, Sch Architecture & Built Environm, Delft, Netherlands
基金
中国国家自然科学基金;
关键词
Perfluorooctanoic acid; Porous activated carbon; Nitrogen-doped activated carbon; Peroxymonosulfate; Thermal activation; PERFLUOROALKYL SUBSTANCES; PERSULFATE ACTIVATION; ORGANIC POLLUTANTS; ELECTRO-FENTON; DEGRADATION; OXIDATION; SOIL; REMEDIATION; MECHANISM; OXYGEN;
D O I
10.1016/j.cej.2020.125722
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The chemical degradation performance of perfluorooctanoic acid (PFOA), one of the environmentally persistent contaminants, by fresh activated carbon (FAC) and nitrogen-doped activated carbon (NAC) which were used as heterogeneous catalysts in the presence of thermal activating peroxymonosulfate (PMS) were investigated and compared. In this study, the physicochemical properties of FAC and NAC are characterized by scanning electron microscope, Raman spectra, Fourier transform infrared spectra, X-ray photoelectron spectroscopy, and Brunauer Emmett Teller. Furthermore, the dosing amount of catalyst, the concentration of oxidant and the effect of catalytic oxidation are investigated. During the catalytic oxidation process, the concentrations of PFOA and its degradation products are determined by high-performance liquid chromatography combined with tandem mass spectrometry (HPLC-MS/MS). The mineralization efficiency of PFOA employing FAC and NAC coupled with thermal activation of PMS are evaluated via a combination approach of total organic carbon (TOC) and ion chromatography (IC). The results indicate that PFOA can be readily degraded at 60 degrees C with an optimum concentration of PMS and an appropriate dosage of FAC/NAC. During the degradation process FAC and NAC exhibit superior adsorption and catalytic performance as more acidic oxygen functional groups are obtained from surface modification, which can facilitate the decomposition of PMS and the mineralization of PFOA. Electron paramagnetic resonance detection confirms that both (OH)-O-center dot and SO4 center dot- exist during oxidation. Based on the identified products, a reaction pathway including adsorption, hydroxylation, and catalytic oxidation is proposed. The methods could not only be applied in a wide pH range to effectively remove PFOA, FAC/PMS and NAC/PMS could also be reused, which provide a feasible and cost-effective method for the degradation of PFOA in situ actual ground water remediation.
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页数:10
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