期刊
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
卷 254, 期 -, 页码 35-44出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.jphotochem.2013.01.003
关键词
Atenolol; Photocatalysis; Kinetics; Intermediates; Degradation pathways
资金
- National Natural Science Foundation of China [20977045, 21177056]
- Fundamental Research Funds for the Central Universities [1112021101]
- China Scholarship Council (CSC)
Photocatalytic degradation of atenolol (ATL) was investigated in aqueous suspensions using TiO2 as photocatalyst. Complete degradation of 37.6 mu M ATL was obtained after 60 min irradiation in pH 6.8 Milli-Q water in the presence of 2.0 g L-1 Degussa P25 TiO2. Degradation of ATL followed pseudo-first-order reaction kinetics. Hydroxyl radical (HO center dot) was determined to be the predominant reactive species during photocatalysis by means of radical probes. Major transformation products were elucidated by high performance liquid chromatograph-mass spectrometry (HPLC-MS/MS) technique. ATL photodegradation pathways included generation of 3-(isopropylamino)propane-1,2-diol and p-hydroxyphenylacetamide through ether chain cleavage, hydroxylation and the formation of 4-[2-hydroxy-3-(isopropylamino)propoxy] benzaldehyde. Frontier electron densities calculation verified the formation of mono-hydroxylation products with HO center dot primarily attacking on benzene ring, which is in agreement with LC-MS/MS analysis. Five carboxylic acids, i.e., oxalic, glyoxylic, malonic, oxamic and formic acids were identified by ion exchange chromatography by comparison with authentic standards. Photocatalytic degradation efficiency of ATL was highly dependent on the properties of the water matrix, such as pH, the presence of organic and inorganic species (e.g., humic substance, HCO3-). River water matrix was found to play a detrimental effect on ATL photocatalytic degradation with a longer irradiation time required for complete elimination of mother compound and intermediate products. Degussa P25 exhibited the highest photocatalytic activity for oxidizing ATL as well as intermediates compared to Aldrich rutile, Millennium PC500 and Hombikat UV100. (C) 2013 Elsevier BM. All rights reserved.
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