Reactive Nitrogen Species Mediated Degradation of Estrogenic Disrupting Chemicals by Biochar/Monochloramine in Buffered Water and Synthetic Hydrolyzed Urine.
Reactive Nitrogen Species Mediated Degradation of Estrogenic Disrupting Chemicals by Biochar/Monochloramine in Buffered Water and Synthetic Hydrolyzed Urine.
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DOI：
10.1021/acs.est.9b04704
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发表时间：
2019-10
影响因子：
11.4
通讯作者：
Zijian Wang;Peizhe Sun;Yaxiu Li;Tan Meng;Zhipeng Li;Xu Zhang;Ruochun Zhang;Hanzhong Jia;H. Yao
中科院分区：
文献类型：
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作者：
Zijian Wang;Peizhe Sun;Yaxiu Li;Tan Meng;Zhipeng Li;Xu Zhang;Ruochun Zhang;Hanzhong Jia;H. Yao
由于雌激素干扰物(EDCs)排放到自然环境中，与内分泌相关的严重健康问题日益引起人们的关注。在这项研究中，我们研究了生物炭(棉花秸秆在350℃下热解棉花秸秆(Cot350)、小麦秸秆在350℃和700℃下热解(WS350和WS700)以及玉米秸秆在350℃和700℃下热解(CS350和CS700)对一氯胺(NH_2Cl)的活化作用，以降解雌二醇(E_2)和乙炔雌二醇(E_2)。在缓冲溶液中，CoT350/NH_2Cl可去除约95%的母体E_2和E_2，24 h内尿液中E_2和E_2的清除率分别为87%和75%。电子顺磁共振分析和自由基猝灭实验表明，生物炭活化了NH_2Cl，并主要生成·NO自由基来降解内皮细胞。CoT350的氮和硅元素是NH_2Cl活化的主要催化中心，而WS700和CS700上的sp2杂化碳起主要作用。分析了尿液中主要成分(氨态氮、氯化物和碳酸氢盐)对生物炭/NH_2Cl反应途径的影响。这项研究为生物炭活化NH_2Cl的反应途径提供了新的见解，并建议了其他碳质材料在活化NH_2Cl方面的潜在应用。
There is increasing concern about the severe endocrine-related health problems due to the discharge of estrogenic disrupting chemicals (EDCs) into the natural environment. In this study, we investigated the activation of monochloramine (NH2Cl) by biochar (pyrolyzed by cotton straw at 350 ℃ (Cot350), wheat straw at 350 ℃ and 700 ℃ (WS350 & WS700), and corn straw at 350 ℃ and 700 ℃ (CS350 & CS700)) for the degradation of estradiol (E2) and ethinylestradiol (EE2). Approximately 95% of parent E2 and EE2 was removed by Cot350/NH2Cl in buffered solution, and 87% of E2 and 75% of EE2 were removed in urine within 24 h. Electronic paramagnetic resonance analysis and radical-quenching experiments showed that biochar activated NH2Cl and primarily generated •NO radicals for the degradation of the EDCs. The nitrogen and silicon elements of Cot350 served as primary catalytic sites for NH2Cl activation, whereas the sp2-hybridized carbon on WS700 and CS700 played a major role. The effect of major urine components (i.e. ammonia species, chloride, and bicarbonate) on the reaction pathways of biochar/NH2Cl was also elucidated. This study provides new insights into the reaction pathways of NH2Cl activation by biochar and suggests potential applications for other carbonaceous materials for NH2Cl activation.