期刊
CHEMOSPHERE
卷 306, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2022.135439
关键词
Polydopamine; GraphiticN; Carbonylgroups; Singletoxygen; Electrontransferprocess
资金
- National Key Research and Devel- opment Program of China [2020YFC1807600]
- National Natural Science Foundation of China [42177072]
The preparation of carbonized polydopamine-decorated g-C3N4 composite material for activation of peroxymonosulfate (PMS) to degrade norfloxacin has achieved excellent catalytic performance. The degradation of norfloxacin is not hindered by sulfate radical and hydroxyl radical, with singlet oxygen and mediated electron transfer identified as the primary mechanisms. The carbonyl group serves as an important active site, and the electron transfer pathway involves adsorption of PMS on the composite material surface and subsequent electron transfer between norfloxacin and the metastable complex.
The use of metal-free graphite carbon nitride (CN) to activate peroxymonosulfate (PMS) has attracted extensive attention for organic pollutants degradation. In this work, we prepared carbonized polydopamine-decorated g-C3N4 (CP-700) for activation of PMS to degrade norfloxacin (NOR). The CP-700 composite was obtained by using CN as a base material on which dopamine underwent an autopolymerization reaction to form a CN-PDA complex, followed by pyrolysis. The apparent porous structure and graphitization provided a large number of active sites for catalytic degradation, enabling CP-700 to exhibit excellent catalytic performance during PMS activation. The degradation of NOR was not hindered by sulfate radical (SO4 center dot-) and hydroxyl radical (center dot OH). Singlet oxygen (O-1(2)) and mediated electron transfer were ultimately identified as the primary mechanisms. According to the linear positive correlation (R-2 = 0.9922) between the semi-quantitative carbonyl group (C=O) and the reaction rate constant, it was determined that the carbonyl group served as the important active site. The excellent electron transfer ability of CP-700 was evidenced by electrochemical techniques and the electron transfer pathway in the system was that PMS was adsorbed on the CP-700 surface to form metastable complex, and then the electron transfer between NOR and metastable complex was achieved. Based on the non-radical pathway, CP-700/PMS system showed a high tolerance to solution pH (3.0-11.0) and inorganic anions. The cyclic degradation
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