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砷酸盐和铬酸盐在水铁矿、菱铁矿和针铁矿纳米结构矿物上的螯合作用:流动反应器实验和 XAS 测量的等温线。

Arsenite and chromate sequestration onto ferrihydrite, siderite and goethite nanostructured minerals: Isotherms from flow-through reactor experiments and XAS measurements.

机构信息

Natural Water Treatment Laboratory, Water Researches and Technologies Center (CERTE), Technopark of Borj-Cedria, PO Box 273, Soliman, 8020, Tunisia.

University Grenoble Alpes, CNRS, ISTerre, CS 40700, F-38058, Grenoble Cedex 9, France.

出版信息

J Hazard Mater. 2019 Jan 15;362:358-367. doi: 10.1016/j.jhazmat.2018.09.031. Epub 2018 Sep 14.

Abstract

Sorption isotherms remain a major tool to describe and predict the mobility of pollutants in natural and anthropogenic environments, but they are typically determined by independent batch experiments. In the present study, the sequestration of As(III), Cr(VI) and competitive As(III)-Cr(VI) on/in 6L-ferrihydrite, siderite and goethite nanostructured minerals was reinvestigated using stirred flow-through reactor experiments. Herein, sorption isotherms were particularly determined from breakthrough curves for inert and reactive tracers monitored simultaneously in a single percolation experiment. In complement, X-ray absorption spectroscopy (XAS) was used to identify As sorption sites on 6L-ferrihydrite and goethite. As expected, the minerals have high potential to remove As and Cr from water (siderite = ferrihydrite (about 60 mg/g) > goethite (20 mg/g)). As and Cr sorption isotherms were modelled with a Langmuir model, and with a sigmoidal Hill model in the case of the competitive sorption. XAS measurements have revealed that As(III) was partially oxidized (up to 22%) in the competitive system with chromate oxyanion Cr(VI). As(III) sorbed on ferrihydrite and goethite adopted edge-sharing and corner sharing complex geometries. Nowadays, a new class of adsorbing phases is being developed for wastewater treatment, including engineered nanostructured materials and nanocomposites. The use of flow through reactor experiments as a high throughput method, combined with XAS, should be considered as efficient screening methods to test their sorbing properties on various contaminants.

摘要

吸附等温线仍然是描述和预测污染物在自然和人为环境中迁移的主要工具,但它们通常是通过独立的批量实验来确定的。在本研究中,使用搅拌流动通过反应器实验重新研究了 6L-水铁矿、菱铁矿和针铁矿纳米结构矿物对 As(III)、Cr(VI)和竞争性 As(III)-Cr(VI)的螯合作用。在此,通过在单个渗滤实验中同时监测惰性和反应性示踪剂的穿透曲线,特别是确定了吸附等温线。此外,还使用 X 射线吸收光谱 (XAS) 来确定 6L-水铁矿和针铁矿上的 As 吸附位点。正如预期的那样,这些矿物具有从水中去除 As 和 Cr 的高潜力(菱铁矿 = 水铁矿(约 60mg/g)> 针铁矿(20mg/g))。使用 Langmuir 模型和竞争吸附情况下的 sigmoidal Hill 模型对 As 和 Cr 吸附等温线进行了建模。XAS 测量表明,在与铬酸盐氧阴离子 Cr(VI)的竞争体系中,As(III)被部分氧化(高达 22%)。在水铁矿和针铁矿上吸附的 As(III)采用边缘共享和角共享复杂几何形状。如今,正在开发一类新的用于废水处理的吸附相,包括工程纳米结构材料和纳米复合材料。作为高通量方法,将流动通过反应器实验与 XAS 结合使用,应该被认为是测试它们对各种污染物的吸附性能的有效筛选方法。

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