Efficient removal of several estrogens in water by Fe-hydrochar composite and related interactive effect mechanism of H2O2 and iron with persistent free radicals from hydrochar of pinewood.
Efficient removal of several estrogens in water by Fe-hydrochar composite and related interactive effect mechanism of H2O2 and iron with persistent free radicals from hydrochar of pinewood.
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DOI：
10.1016/j.scitotenv.2018.12.183
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发表时间：
2019-03
期刊：
影响因子：
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通讯作者：
Jianan Yu;Zhiliang Zhu;Hua Zhang;Ting Chen;Y. Qiu;Zhaoyi Xu;D. Yin
中科院分区：
文献类型：
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作者：
Jianan Yu;Zhiliang Zhu;Hua Zhang;Ting Chen;Y. Qiu;Zhaoyi Xu;D. Yin
近年来，具有持久性自由基（PFRs）的碳氢化合物（HC）在非均相类芬顿反应中的潜在应用受到了研究人员的关注，但关于H2O2、铁和HC在去除有机污染物中的相互作用的研究仍然有限。以松木水热炭为原料合成了磁性铁（水）氧化物固定化碳氢化合物（Fe/HC），并对其进行了表征。系统研究了H2O2、铁和HC在去除几种雌激素中的交互作用，特别是在接近自然水环境的pH范围内，了解了它们的去除性能和相关机制。批量实验结果表明，在4 ~ 9的较宽pH范围内，Fe/HC材料能有效去除雌激素。基于电子自旋共振、x射线光电子能谱、Mössbauer能谱和电化学阻抗谱分析，机理研究表明，碳氢化合物表面的碳心PFRs可以作为电子供体，将吸附在o2上的电子快速转移生成自由基dotO2−，而h2o2的加入增强了电子在材料表面产生自由基dotO2 （ads）的传输能力。铁和碳氢化合物组分通过催化和吸附之间的协同作用有助于理想的去除雌激素。本研究为铁/HC材料在水环境中微量雌激素污染的修复提供了广阔的应用前景。
Recently, hydrochar (HC) with existed persistent free radicals (PFRs) has attracted researches' attention for the potential application in heterogeneous Fenton-like reactions, but studies on the interactive effects of H2O2, iron, and HC in removal of organic pollutants are still limited. In this paper, magnetic iron (hydr)oxides immobilized hydrochar composite (Fe/HC) derived from hydrothermal carbon (HTC) of pinewood were synthesized and characterized. The interactive effects of H2O2, iron, and HC in the removal of several estrogens were systematically investigated to understand the removal performance and related mechanism, especially at a pH range close to natural water environment. Batch experiments results showed that estrogens could be efficiently removed over Fe/HC material under a wide pH range of 4–9. Based on the analysis of electron spin resonance, X-ray photoelectron spectroscopy, Mössbauer spectroscopy, and electrochemical impedance spectroscopy, mechanism study indicated that the carbon-centered PFRs on the surface of hydrochar can act as electron donors, and transfer the electrons on adsorbed O2to generate radical dotO2−rapidly, while the addition of H2O2enhanced the transmission ability of electron to produce radical dotOH(ads)on the material surface. The iron and hydrochar components contributed to the desirable removal of estrogens via the synergistic effect between catalysis and adsorption. This study provides a promising application for the use of Fe/HC materials on remediation of pollution with trace estrogens in water environment.