纳米零价铁降解水中17β-雌二醇的作用机制

doi:10.16085/j.issn.1000-6613.2019-1975

摘要/Abstract

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?O $2 -$ 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?O $2 -$ 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。

关键词: 17β-雌二醇, 纳米零价铁, 降解机理, 活性氧物质

Abstract:

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 ?O $2 -$ , and as pH increased, the dominant position of ?OH was gradually replaced by ?O $2 -$ . The degradation efficiency and rate of 17β-E2 were positively correlated with the yield and production rate of Fe²⁺ 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 of 17β-E2. The experimental results provided theoretical support for the repair of estrogen-contaminated water and the directional optimization of nZVI.

Key words: 17β-estradiol, nano-zero valent iron, degradation mechanism, reactive oxygen species

中图分类号:

X703

杨硕, 余薇薇, 杨伦, 杜邦昊, 谢明原, 赵晨菊, 万巧玲, 潘伟亮. 纳米零价铁降解水中17β-雌二醇的作用机制[J]. 化工进展, 2020, 39(9): 3826-3834.

Shuo YANG, Weiwei YU, Lun YANG, Banghao DU, Mingyuan XIE, Chenju ZHAO, Qiaoling WAN, Weiliang PAN. Degradation mechanism of 17β-estradiol by nano-zero valent iron in aqueous solution[J]. Chemical Industry and Engineering Progress, 2020, 39(9): 3826-3834.

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