Enhanced Radical Generation in an Ultraviolet/Chlorine System through the Addition of TiO2
Autor: | Zhuo-Yu Li, Xiaohui Lu, Hao-Chen Zhang, Tao Yang, Yulei Liu, Jun Ma, Lu Wang |
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Rok vydání: | 2021 |
Předmět: |
Aqueous solution
Radical Advanced oxidation process chemistry.chemical_element General Chemistry medicine.disease_cause Photochemistry Chemical kinetics chemistry.chemical_compound chemistry polycyclic compounds Chlorine medicine Environmental Chemistry Reactivity (chemistry) Dimethyl phthalate Ultraviolet |
Zdroj: | Environmental Science & Technology. 55:11612-11623 |
ISSN: | 1520-5851 0013-936X |
DOI: | 10.1021/acs.est.0c08785 |
Popis: | Ultraviolet (UV)/chlorine draws increasing attention for the abatement of recalcitrant organic pollutants. Herein, it was found that TiO2 would significantly promote the degradation of dimethyl phthalate (DMP) in the UV/chlorine system (from 19 to 84%). Hydroxyl radicals (HO•) and chlorine radicals (Cl•) were the dominant reactive species for DMP degradation in the UV/chlorine/TiO2 system. Chlorine decayed much faster in UV/chlorine/TiO2 compared with UV/chlorine, which is possibly because photogenerated electrons (ecb-) and superoxide radicals (O2•-) have high reactivity with chlorine. As a result, the recombination of photogenerated holes (hvb+) and ecb- was inhibited and the accumulation of HO• and Cl• was facilitated. A kinetic model was established to simulate the reaction process, and it was found that the concentrations of HO• and Cl• were several times to dozens of times higher in UV/chlorine/TiO2 than that in UV/chlorine. The contributions of HO• and Cl• to DMP degradation were 70.3 and 29.7% by model simulation, respectively, and were close to the probe experiment result. In the UV/chlorine/TiO2 system, the degradation of DMP did not follow pseudo-first-order kinetics but the degradation of benzoate fitted well with pseudo-first-order kinetics. This phenomenon was elucidated by the structure of the pollutant and TiO2 and further tested by calculating the adsorption energy (Eads)/binding energy (Eb) with density functional theory. Due to faster decay of chlorine, lower amounts of disinfection byproducts formed in UV/chlorine/TiO2 compared with UV/chlorine. Adding TiO2 into the UV/chlorine system can promote the degradation of recalcitrant organic pollutants in an aqueous environment. |
Databáze: | OpenAIRE |
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