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.
机构:
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences
Central South China Center for Geoscience InnovationState Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences
Caixiang Zhang
Xiaoping Liao
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State Key Laboratory of Biogeology and Environmental Geology, China University of GeosciencesState Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences
Xiaoping Liao
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机构:
You Lü
Chao Nan
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机构:
State Key Laboratory of Biogeology and Environmental Geology, China University of GeosciencesState Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences
机构:
Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Natl Engn Res Ctr Urban Water Resources, Harbin 150090, Peoples R ChinaHarbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Zhao, Ji
Yang, Jingjing
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Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Suzhou Univ Sci & Technol, Ctr Separat & Purificat Mat & Technol, Suzhou 215009, Peoples R ChinaHarbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Yang, Jingjing
Ma, Jun
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Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Natl Engn Res Ctr Urban Water Resources, Harbin 150090, Peoples R ChinaHarbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China