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纳米零价铁去除磺胺甲恶唑的评估。

Assessment of sulfamethoxazole removal by nanoscale zerovalent iron.

机构信息

Research Institute of Sciences and Engineering, University of Sharjah, Sharjah, United Arab Emirates; Department of Civil and Environmental Engineering, University of Sharjah, Sharjah, United Arab Emirates.

Department of Civil and Environmental Engineering, University of Sharjah, Sharjah, United Arab Emirates.

出版信息

Sci Total Environ. 2021 Mar 20;761:143307. doi: 10.1016/j.scitotenv.2020.143307. Epub 2020 Nov 3.

Abstract

Removal of pharmaceutical compounds, such as sulfamethoxazole (SMX) from the aquatic environments, is critical in order to mitigate their adverse environmental and human health effects. In this study, the effectiveness of nanoscale zerovalent iron (nZVI) particles for the removal of SMX was investigated under varying conditions of initial solution pH (3, 5, 7 and 11) and nZVI to SMX mass ratios (1:1, 5:1, 10:1, 13:1, 25:1). Batch kinetic studies, which were well represented using both pseudo-first-order and pseudo-second-order kinetic models (R > 0.98), showed that both solution pH and mass ratios strongly influenced SMX removal. At a fixed mass ratio of 10:1, removal efficiencies were higher in acidic conditions (83% to 91%) compared to neutral (29%) and alkaline (6%) conditions. A similar trend was observed for removal rates and removal amounts. For mass ratios between 1:1 and 10:1, an optimum pH existed (pH 5) wherein highest removal efficiencies were attained. Increasing the mass ratio above 10:1 resulted in virtually complete removal efficiencies at pH 3 and 5, and 70% at pH 7. Analysis of SMX speciation and zeta potential of nZVI particles provided insights into the role of pH on the efficiencies, rates and extents of SMX removal. Total organic carbon analysis and mass spectrometry measurements of SMX solution before and after exposure to nZVI particles suggested the transformation of SMX via redox reactions, which are likely the dominant process compared to adsorption. Five transformation products were observed at m/z 156 (TP1), 192 (TP2), 256 (TP3), 294 (TP4) and 296 (TP5). TP1, TP2 and TP3 were further identified using ion fragment analysis. Overall, results from this study indicate a strong potential for SMX removal by nZVI particles, and could be useful towards identifying reaction conditions for optimum SMX transformation.

摘要

从水环境中去除磺胺甲恶唑 (SMX) 等药物化合物对于减轻其对环境和人类健康的不利影响至关重要。本研究考察了纳米零价铁 (nZVI) 颗粒在不同初始溶液 pH 值 (3、5、7 和 11) 和 nZVI 与 SMX 质量比 (1:1、5:1、10:1、13:1、25:1) 条件下对 SMX 的去除效果。批处理动力学研究表明,两种动力学模型(准一级和准二级动力学模型)均能很好地描述反应过程 (R>0.98),结果表明溶液 pH 值和质量比对 SMX 的去除均有强烈影响。在固定质量比为 10:1 的条件下,酸性条件下的去除效率较高 (83% 至 91%),中性 (29%) 和碱性 (6%) 条件下的去除效率较低。去除速率和去除量也表现出类似的趋势。对于质量比在 1:1 和 10:1 之间,存在最佳 pH 值 (pH 5),此时可以获得最高的去除效率。当质量比超过 10:1 时,在 pH 3 和 5 时几乎可以实现完全去除效率,在 pH 7 时可以实现 70%的去除效率。SMX 形态分析和 nZVI 颗粒的zeta 电位分析为 pH 值对去除效率、速率和程度的影响提供了深入的见解。SMX 溶液在暴露于 nZVI 颗粒前后的总有机碳分析和质谱测量表明,SMX 通过氧化还原反应发生转化,与吸附相比,这可能是主要过程。在 m/z 156 (TP1)、192 (TP2)、256 (TP3)、294 (TP4) 和 296 (TP5) 处观察到五个转化产物。通过离子碎片分析进一步鉴定了 TP1、TP2 和 TP3。总的来说,本研究结果表明 nZVI 颗粒对 SMX 具有很强的去除潜力,可为确定最佳 SMX 转化的反应条件提供有用信息。

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