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采用颗粒铁和有机碳处理缺氧地下水中 Se(VI)的机理研究:EXAFS 研究。

Mechanistic investigations of Se(VI) treatment in anoxic groundwater using granular iron and organic carbon: an EXAFS study.

机构信息

Department of Earth and Environmental Sciences, University of Waterloo, 200 University Ave. W., Waterloo, ON N2L 3G1, Canada.

出版信息

J Hazard Mater. 2012 Nov 30;241-242:92-100. doi: 10.1016/j.jhazmat.2012.09.015. Epub 2012 Sep 16.

Abstract

The removal of aqueous Se(VI) from a simulated groundwater by granular iron (GI), organic carbon (OC), and a mixture of these reactive materials (GI-OC) was evaluated in laboratory batch experiments. The experiments were performed under anoxic conditions to simulate subsurface treatment. A total reaction time of 120 h (5 d) was chosen to investigate the rapid changes in speciation occurring over reaction times that are reasonable for permeable reactive barrier (PRB) systems. After 120 h, concentrations of Se decreased by >90% in the GI system, 15% in the OC system and 35% in the GI-OC mixture. Analysis of the materials after contact with Se using synchrotron-radiation based X-ray absorption spectroscopy (XAS) indicated the presence of Se(IV) and Se(0) on the margins of GI grains after 6h with evidence of SeO and SeSe bonding, whereas Se(VI) was not observed. After 72 h, Se(0) was the only form of Se present in the GI experiments. In the OC batches, the XAS analysis indicated binding consistent with sorption of aqueous Se(VI) onto the OC with only minor reduction to Se(IV) and Se(0) after 120 h. Selenium XAS spectra collected for the GI-OC mixture were consistent with spectra for Se(IV) and Se(0) on both the margins of GI grains and OC particles, suggesting that the presence of dissolved Fe may have mediated the reduction of sorbed Se(VI). The results suggest that the application of granular Fe is effective at inducing aqueous Se removal in anoxic conditions through reductive precipitation processes.

摘要

实验室批量实验评估了颗粒铁(GI)、有机碳(OC)和这些反应性材料的混合物(GI-OC)从模拟地下水中去除六价硒的效果。实验在缺氧条件下进行,以模拟地下处理。选择总反应时间为 120 h(5 d),以研究在合理的可渗透反应屏障(PRB)系统的反应时间内发生的形态快速变化。120 h 后,GI 体系中硒的浓度降低了>90%,OC 体系中硒的浓度降低了 15%,GI-OC 混合物中硒的浓度降低了 35%。用基于同步辐射的 X 射线吸收光谱法(XAS)对与硒接触后的材料进行分析表明,在 6 h 后,GI 颗粒边缘存在 Se(IV)和 Se(0),并有 SeO 和 SeSe 键合的证据,而未观察到 Se(VI)。72 h 后,GI 实验中仅存在 Se(0)这一种硒形态。在 OC 批次中,XAS 分析表明,在 120 h 后,吸附在 OC 上的六价硒主要以 Se(IV)和 Se(0)的形式存在,结合情况一致。GI-OC 混合物的硒 XAS 光谱与 GI 颗粒边缘和 OC 颗粒上的 Se(IV)和 Se(0)的光谱一致,表明溶解的 Fe 的存在可能介导了吸附的 Se(VI)的还原。结果表明,在缺氧条件下,颗粒铁的应用通过还原沉淀过程有效地诱导了水中硒的去除。

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