Citation: Zhu Benzhan, Shao Bo, Mao Li, Gao Huiying. Intrinsic Chemiluminescence Production during Environmentally-friendly Advanced Oxidation of Halogenated Aromatics and Its Applications[J]. Acta Chimica Sinica, ;2016, 74(7): 557-564. doi: 10.6023/A16040178 shu

Intrinsic Chemiluminescence Production during Environmentally-friendly Advanced Oxidation of Halogenated Aromatics and Its Applications

1.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China

Corresponding author: Zhu Benzhan, bzhu@rcees.ac.cn
Received Date: 11 April 2016
Revised Date: 23 May 2016

Fund Project: National Natural Science Foundation of China 21577149Strategic Priority Research Program of CAS XDB01020300National Natural Science Foundation of China 21321004Open Foundation from State Key Laboratory of Environmental Chemistry and Ecotoxicology KF2012-09National Natural Science Foundation of China 21477139National Natural Science Foundation of China 21237005

Figures(7)

Haloaromatics (XAr) have been widely used as pesticides, personal care agents, pharmaceuticals and flame retardants, which are now ubiquitously present in our environment. The carcinogenicity coupled with their ubiquitous occurrence have raised public concerns on the potential risks to both human health and the ecosystem posed by XAr. Advanced oxidation processes (AOPs) have been increasingly employed as an "environmentally-friendly" technology for remediating such highly toxic and recalcitrant XAr. During these AOPs systems, the most reactive radical intermediate formed at near-ambient temperature and pressure is the hydroxyl radical (^·OH). Recently, we found that an intrinsic chemiluminescence can be generated during the advanced oxidation of the priority pollutant pentachlorophenol and all other XAr. Furtherly, by the complementary application of electron spin resonance (ESR) with 5, 5-dimethyl-1-pyrroline-N-oxide (DMPO) as the spin-trapping agent, fluorescence method with terephthalic acid (TPA) as the ^·OH probe, chemiluminescence analysis in the presence of classic ^·OH scavengers and several typical ^·OH-generating systems, the chemiluminescence was confirmed to be directly dependent on the production of the extremely reactive ^·OH. Further studies showed that halogenated quinoid intermediates were produced during the degradation of XAr by ^·OH-generating system, which could produce weak chemiluminescence that was greatly enhanced by addition of extra ^·OH. We proposed that this unusual chemiluminescence generation was due to hydroxyl radical-dependent production of halogenated quinoid intermediates and electronically excited carbonyl species. In addition, the time course of chemiluminescence emission correlated well with the degradation of XAr: when the degradation level of XAr reached the maximum, no further chemiluminescence emission could be observed. Based on these findings, we developed a rapid, sensitive, simple, and effective chemiluminescence method to not only measure trace amount of XAr, but also monitor their real-time degradation kinetics. These new findings may have broad chemical, pharmaceutical, toxicological and environmental implications for future studies on remediation of these halogenated persistent organic pollutants by AOPs.
- chemiluminescence,
- halogenated aromatics,
- hydroxyl radicals,
- advanced oxidation processes,
- Fenton and Fenton-like reactions
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