Enhanced Degradation of Micropollutants in a Peracetic Acid/Mn(II) System with EDDS: An Investigation of the Role of Mn Species

被引:8
|
作者
Dong, Jie [1 ,2 ]
Dong, Haoran [1 ,2 ]
Xiao, Junyang [1 ,2 ]
Li, Long [1 ,2 ]
Huang, Daofen [1 ,2 ]
Zhao, Mengxi [1 ,2 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China
[2] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Hunan, Peoples R China
基金
中国国家自然科学基金;
关键词
peracetic acid; EDDS; high-valent manganese-oxospecies; reactive oxygen species; micropollutant; OXIDATIVE-DEGRADATION; ORANGE II; ACID; FENTON; COMPLEXES; MECHANISM; RADICALS; CATALYST; ATRAZINE; IMPACT;
D O I
10.1021/acs.est.4c00901
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Extensive research has been conducted on the utilization of a metal-based catalyst to activate peracetic acid (PAA) for the degradation of micropollutants (MPs) in water. Mn(II) is a commonly employed catalyst for homogeneous advanced oxidation processes (AOPs), but its catalytic performance with PAA is poor. This study showed that the environmentally friendly chelator ethylenediamine-N,N '-disuccinic acid (EDDS) could greatly facilitate the activation of Mn(II) in PAA for complete atrazine (ATZ) degradation. In this process, the EDDS enhanced the catalytic activity of manganese (Mn) and prevented disproportionation of transient Mn species, thus facilitating the decay of PAA and mineralization of ATZ. By employing electron spin resonance detection, quenching and probe tests, and O-18 isotope-tracing experiments, the significance of high-valent Mn-oxo species (Mn(V)) in the Mn(II)-EDDS/PAA system was revealed. In particular, the involvement of the Mn(III) species was essential for the formation of Mn(V). Mn(III) species, along with singlet oxygen (O-1(2)) and acetyl(per)oxyl radicals (CH3C(O)O-center dot/CH3C(O)OO center dot), also contributed partially to ATZ degradation. Mass spectrometry and density functional theory methods were used to study the transformation pathway and mechanism of ATZ. The toxicity assessment of the oxidative products indicated that the toxicity of ATZ decreased after the degradation reaction. Moreover, the system exhibited excellent interference resistance toward various anions and humid acid (HA), and it could selectively degrade multiple MPs.
引用
收藏
页码:12179 / 12188
页数:10
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