化工进展 ›› 2020, Vol. 39 ›› Issue (9): 3826-3834.DOI: 10.16085/j.issn.1000-6613.2019-1975

• 资源与环境化工 • 上一篇    下一篇

纳米零价铁降解水中17β-雌二醇的作用机制

杨硕1(), 余薇薇1(), 杨伦1, 杜邦昊1, 谢明原1, 赵晨菊1, 万巧玲2, 潘伟亮1   

  1. 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
  • 出版日期:2020-09-05 发布日期:2020-09-11
  • 通讯作者: 余薇薇
  • 作者简介:杨硕(1994—),男,硕士研究生,研究方向为水处理。E-mail:alonzoy@foxmail.com
  • 基金资助:
    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)

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

Shuo YANG1(), Weiwei YU1(), Lun YANG1, Banghao DU1, Mingyuan XIE1, Chenju ZHAO1, Qiaoling WAN2, Weiliang PAN1   

  1. 1.School of River and Ocean Engineering, Chongqing Jiaotong University, Key Laboratory of Hydraulic and Waterway Engineering of the Ministry of Education, Chongqing 400074, China
    2.Chongqing Monitoring Station, Water Quality Monitoring Network of National Urban Water Supply, Chongqing 400060, China
  • Online:2020-09-05 Published:2020-09-11
  • Contact: Weiwei YU

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。

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 ?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 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

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