A Fe(II)/citrate/UV/PMS process for carbamazepine degradation at a very low Fe(II)/PMS ratio and neutral pH: The mechanisms

被引:163
作者
Ling, Li [1 ]
Zhang, Dapeng [1 ]
Fan, Chihhao [2 ]
Shang, Chii [1 ,3 ]
机构
[1] Hong Kong Univ Sci & Technol, Dept Civil & Environm Engn, Kowloon, Hong Kong, Peoples R China
[2] Natl Taiwan Univ, Dept Bioenvironm Syst Engn, Taipei, Taiwan
[3] Hong Kong Univ Sci & Technol, Chinese Natl Engn Res Ctr Control & Treatment Hea, Hong Kong Branch, Kowloon, Hong Kong, Peoples R China
关键词
Photo-Fenton-like AOPs; Ferric-citrate complexation; Carbamazepine removal; PPCP; UV; Peroxymonosulfate; ADVANCED OXIDATION PROCESSES; HYDROXYL RADICALS; SPECTROPHOTOMETRIC DETERMINATION; ORGANIC CONTAMINANTS; AQUEOUS-SOLUTION; RATE CONSTANTS; QUANTUM YIELD; PERSULFATE; WATER; UV;
D O I
10.1016/j.watres.2017.07.066
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A novel Fe(II)/citrate/UW/PMS process for degrading a model micropollutant, carbamazepine (CBZ), at a low Fe(II)/PMS ratio and neutral pH has been proposed in this study, and the mechanisms of radical generation in the system was explored. With a UV dose of 302.4 mJ/cm(2), an initial pH of 7, and CBZ, PMS, Fe(II) and citrate at initial concentrations of 10, 100, 12 and 26 mu M, respectively, the CBZ degradation efficiency reached 71% in 20 min in the Fe(II)/citrate/UV/PMS process, which was 4.7 times higher than that in either the citrate/UV/PMS or Fe(II)/citrate/PMS process. The enhanced CBZ degradation in the Fe(II)/citrate/UV/PMS process was mainly attributed to the continuous activation of PMS by the UV catalyzed regenerated Fe(II) from a Fe(III)-citrate complex, [Fe3O(cit)(3)H-3](2-), which not only maintained Fe(III) soluble at, neutral pH, but also increased 6.6 and 2.6 times of its molar absorbance and quantum yield as compared to those of ionic Fe(III), respectively. In the Fe(II)/citrate/UV/PMS process, the SO4 center dot- produced from the fast reaction between PMS and the initially-added Fe(II) contributed 11% of CBZ degradation. The PMS activation by the UV radiation and regenerated Fe(II) contributed additional 14% and 46% of CBZ removal, respectively. The low iron and citrate doses and the fast radical generation at neutral pH make the Fe(II)/citrate/UV/PMS process suitable for degrading recalcitrant organic compounds in potable water. (C) 2017 Elsevier Ltd. All rights reserved.
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页码:446 / 453
页数:8
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