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天然有机物对 KCl 和 CaCl2 溶液中 CeO2 纳米颗粒聚集动力学的影响:测量和模拟。

Effect of natural organic matter on the aggregation kinetics of CeO2 nanoparticles in KCl and CaCl2 solutions: measurements and modeling.

机构信息

School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.

出版信息

J Hazard Mater. 2012 Mar 30;209-210:264-70. doi: 10.1016/j.jhazmat.2012.01.013. Epub 2012 Jan 12.

Abstract

To characterize the environmental transport and quantify the risk of nanoparticles (NPs), it is important to fundamentally understand the aggregation of NPs and to describe this process quantitatively. This study investigates the aggregation kinetics of CeO(2) NPs in the presence of KCl, CaCl(2) and humic acid (HA) using time-resolved dynamic light scattering. In KCl solutions, regardless of their concentration, HA drastically reduces the aggregation kinetics of CeO(2) NPs. However, the effect of HA was more complicated in CaCl(2) solutions. At low CaCl(2) concentrations, HA inhibited NP aggregation, whereas at high CaCl(2) concentrations, HA promoted aggregation. The critical coagulation concentration (CCC) in KCl in the absence of HA is approximately 36.5mM. In presence of both 1 ppm and 10 ppm HA in KCl solutions, extremely low aggregation kinetics were observed even at very high KCl concentrations (500 mM), implying KCl-CCCs in presence of HA were larger than 500 mM. The CCCs under conditions of no HA, 1 ppm HA and 10 ppm HA in CaCl(2) solutions are approximately 9.5, 8.0 and 12.0mM, respectively. These observations were analyzed in the framework of extended Derjaguin-Landau-Verwey-Overbeek (EDLVO) theory. Moreover, a kinetic model was used to predict the aggregation kinetics of CeO(2) NPs. The model predictions are in close agreement with experimental observations. To the best of our knowledge, this work is the first to model quantitatively the aggregation of NPs in the presence of natural organic matter.

摘要

为了描述纳米粒子(NPs)的环境传输并量化其风险,重要的是要从根本上理解 NPs 的聚集并对其进行定量描述。本研究使用时间分辨动态光散射研究了 CeO(2) NPs 在 KCl、CaCl(2) 和腐殖酸(HA)存在下的聚集动力学。在 KCl 溶液中,无论其浓度如何,HA 都会大大降低 CeO(2) NPs 的聚集动力学。然而,HA 的影响在 CaCl(2)溶液中更为复杂。在低 CaCl(2)浓度下,HA 抑制 NP 聚集,而在高 CaCl(2)浓度下,HA 促进聚集。不存在 HA 时 KCl 中的临界聚沉浓度(CCC)约为 36.5mM。在 KCl 溶液中存在 1ppm 和 10ppm HA 的情况下,即使在非常高的 KCl 浓度(500mM)下,也观察到非常低的聚集动力学,这意味着存在 HA 时 KCl-CCC 大于 500mM。在不存在 HA、1ppm HA 和 10ppm HA 的条件下,CaCl(2)溶液中的 CCC 分别约为 9.5、8.0 和 12.0mM。这些观察结果是在扩展的 Derjaguin-Landau-Verwey-Overbeek(EDLVO)理论框架内进行分析的。此外,还使用动力学模型来预测 CeO(2) NPs 的聚集动力学。模型预测与实验观察结果非常吻合。据我们所知,这项工作是首次定量地模拟 NPs 在天然有机物存在下的聚集。

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