纳米零价铁降解水中17β-雌二醇的作用机制  

Degradation mechanism of 17β-estradiol by nano-zero valent iron in aqueous solution

作　　者：杨硕 余薇薇 杨伦 杜邦昊 谢明原 赵晨菊 万巧玲 潘伟亮 YANG Shuo;YU Weiwei;YANG Lun;DU Banghao;XIE Mingyuan;ZHAO Chenju;WAN Qiaoling;PAN Weiliang(School of River and Ocean Engineering,Chongqing Jiaotong University,Key Laboratory of Hydraulic and Waterway Engineering of the Ministry of Education,Chongqing 400074,China;Chongqing Monitoring Station,Water Quality Monitoring Network of National Urban Water Supply,Chongqing 400060,China)

机构地区：[1]重庆交通大学河海学院,水利水运工程教育部重点实验室,重庆400074 [2]国家城市供水水质监测网重庆监测站,重庆400060

出　　处：《化工进展》2020年第9期3826-3834,共9页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(51608079);重庆交通大学河海学院研究生教育创新基金(YC2019008);国家内河航道整治工程技术研究中心暨水利水运工程教育部重点实验室开放基金(SLK2018A04);重庆市研究生教育教学改革研究项目(重点项目)(yig182028)。

摘　　要：为探究纳米零价铁(nZVI)对水中17β-雌二醇(17β-E2)的降解机制和降解路径,本研究采用降解动力学拟合分析不同初始pH (3、5和7)对17β-E2降解过程的影响。结果表明,酸性条件下17β-E2可被nZVI高效降解,而中性条件下其降解受到极大限制。随着pH进一步降低,nZVI的降解17β-E2的能力仅从降解速率上提升而非降解效率。·OH和·O2^-在降解过程中占据主导地位,且随着pH上升·OH的主导地位逐渐被·O2^-取代。nZVI自身腐蚀下Fe2+产量和产生速率与17β-E2的降解率和降解速率呈正相关。对降解产物的分析表明,17β-E2可在nZVI作用下转化为E1并在酸性条件下被进一步降解;17β-E2的降解路径可归纳为芳香环基团的替换、断裂和开环;降解产物二聚体和三聚体的证实了仿漆酶反应对17β-E2降解的贡献。实验结果为雌激素污染水体的修复以及nZVI的定向优化提供了理论支撑。To investigate the degradation mechanism and the possible degradation pathways of 17β-estradiol(17β-E2) in water by nano-zero valent iron(nZVI).In this study,the degradation kinetics fittings were used to analyze the effects of different initial pH(3,5 and 7) in the degradation process.The result showed that 17β-E2 could be degraded efficiently by nZVI under acidic conditions,but greatly limited under neutral conditions.With the further decrease of pH,the degradation ability of nZVI to 17β-E2 increased from the degradation rate rather than the degradation efficiency.The degradation processes were dominated by ·OH and ·O2^-,and as pH increased,the dominant position of ·OH was gradually replaced by ·O2·.The degradation efficiency and rate of 17β-E2 were positively correlated with the yield and production rate of Fe^2+ by the corrosion of nZVI.Analysis of degradation products showed that 17β-E2 could be converted to E1 by nZVI and further degraded under acidic conditions.The degradation pathways could be attributed to the groups substitution,fragmentation and opening of ring A.Degradation products(dimers and trimers) confirmed the contribution of the laccase-like reaction to the degradation of17β-E2.The experimental results provided theoretical support for the repair of estrogen-contaminated water and the directional optimization of nZVI.

关 键 词：17Β-雌二醇 纳米零价铁 降解机理 活性氧物质 

分 类 号：X703[环境科学与工程—环境工程]