期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 52, 期 11, 页码 6317-6325出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.8b00576
关键词
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资金
- Natural Science Foundation of China [21677181, 51378515]
- National Key Research Development Program of China [2016YFC0502803]
- Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program [2015TQ01Z552]
- Guangzhou Science Technology and Innovation Commission [201707010249]
- Science and Technology Project of Zhejiang Province [2017G33036]
- Fundamental Research Funds for the Central Universities [17lgzd21]
- University of Cincinnati
- Herman Schneider Professorship in the College of Engineering and Applied Sciences
Halides and natural organic matter (NOM) are inevitable in aquatic environment and influence the degradation of contaminants in sulfate radical (SO4 center dot-)-based advanced oxidation processes. This study investigated the formation of chlorate in the coexposure of SO4 center dot-, chloride (Cl-), bromide (Br-) and/or NOM in UV/persulfate (UV/PDS) and cobalt(II)/ peroxymonosulfate (Co/PMS) systems. The formation of chlorate increased with increasing Cl- concentration in the UV/PDS system, however, in the Co/PMS system, it initially increased and then decreased. The chlorate formation involved the formation of hypochlorous acid/hypochlorite (HOCl/OCl-) as an intermediate in both systems. The formation was primarily attributable to SO4 center dot- in the UV/PDS system, whereas Co(III) played a significant role in the oxidation of Cl- to HOCl/OCl- and SO4 center dot- was important for the oxidation of HOCl/OCl- to chlorate in the Co/PMS system. The pseudo-first-order rate constants (k') of the transformation from Cl- to HOCl/OCl- were 3.32 x 10(-6) s(-1) and 9.23 X 10(-3) s(-1) in UV/PDS and Co/PMS, respectively. Meanwhile, k' of HOCl/OCl- to chlorate in UV/PDS and Co/PMS were 2.43 x 10(-3) s(-1) and 2.70 X 10(-4) s(-1), respectively. Br- completely inhibited the chlorate formation in UV/PDS, but inhibited it by 45.2% in Co/PMS. The k' of SO(4)(center dot-)reacting with Br- to form hypobromous acid/hypobromite (HOBr/OBr-) was calculated to be 378 times higher than that of Cl- to HOCl/OCl-, but the k' of Co(III) reacting with Br- to form HOBr/OBr- was comparable to that of Cl- to HOClOCl-. NOM also significantly inhibited the chlorate formation, due to the consumption of SO4 center dot- - and reactive chlorine species (RCS, such as Cl center dot, ClO center dot and HOCl/OCl-). This study demonstrated the formation of chlorate in SO4 center dot- -based AOPs, which should to be considered in their application in water treatment.
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