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From Quencher to Promoter: Revisiting the Role of 2,4,6-Trimethylphenol (TMP) in Triplet-State Photochemistry of Dissolved Organic Matter
被引:0
|作者:
Du, Penghui
[1
,2
,3
]
Yang, Biwei
[1
,2
]
Chow, Alex Tat-Shing
[3
]
Shi, Dongliang
[4
]
Wong, Keith Man-Chung
[4
]
Wang, Junjian
[1
,2
]
机构:
[1] Southern Univ Sci & Technol, Sch Environm Sci & Engn, State Environm Protect Key Lab Integrated Surface, Shenzhen 518055, Guangdong, Peoples R China
[2] Southern Univ Sci & Technol, Sch Environm Sci & Engn, Guangdong Prov Key Lab Soil & Groundwater Pollut C, Shenzhen 518055, Guangdong, Peoples R China
[3] Chinese Univ Hong Kong, Dept Earth & Environm Sci, Hong Kong 999077, Peoples R China
[4] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
基金:
中国国家自然科学基金;
关键词:
photosensitizer;
long-lived photooxidant;
phenoxylradical;
kinetic modeling;
laser flash photolysis;
PROTON-ELECTRON TRANSFERS;
SULFONAMIDE ANTIBIOTICS;
INDUCED TRANSFORMATION;
PHENOXYL RADICALS;
FURFURYL ALCOHOL;
OXIDATION;
REACTIVITY;
DEGRADATION;
WATER;
KINETICS;
D O I:
10.1021/acs.est.4c09859
中图分类号:
X [环境科学、安全科学];
学科分类号:
08 ;
0830 ;
摘要:
Triplet-state dissolved organic matter (3DOM*) plays a crucial role in environmental aquatic photochemistry, with 2,4,6-trimethylphenol (TMP) frequently used as a chemical probe or quencher due to its high reactivity with 3DOM*. However, the influence of TMP-derived oxidation intermediates on the target photochemical reactions has not been comprehensively examined. This study investigated TMP's effect on the photolysis of sulfamethoxazole (SMX), a common antibiotic found in natural waters, in the presence of different DOM sources or model photosensitizer. Contrary to expectation, TMP significantly accelerated SMX photolysis, with the extent of enhancement depending on TMP and DOM concentrations. Laser flash photolysis and kinetic modeling suggested the long-lived TMP-derived reactive species (TMP-RS), including phenoxyl radicals, semiquinone radicals, and quinones, as the key factors in this process. Unlike 3DOM*, TMP-RS may react with SMX with the formation of non-SMX center dot+ intermediates. This process prevents the reduction of SMX center dot+ and the subsequent regeneration of SMX. The kinetic model successfully predicts the dynamic contributions of various factors to SMX oxidation during the reaction, highlighting the critical role of TMP-RS. This study advances our understanding of TMP's involvement in triplet-state photochemistry and suggests a reconsideration of the role long-lived organic RSs play in the transformation of environmental micropollutants.
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页码:4444 / 4454
页数:11
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