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解析 NO、SO 和细胞外聚合物在 CeO 纳米颗粒聚集动力学中的作用:测量与建模。

Interpreting the role of NO, SO, and extracellular polymeric substances on aggregation kinetics of CeO nanoparticles: Measurement and modeling.

机构信息

Key Laboratory of Eco-environments in Three Gorges Reservoir Region, Ministry of Education, College of Environment and Ecology, Chongqing University, China.

State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, 150090, China.

出版信息

Ecotoxicol Environ Saf. 2020 May;194:110456. doi: 10.1016/j.ecoenv.2020.110456. Epub 2020 Mar 12.

Abstract

The early stage of aggregation of cerium oxide nanoparticles (CeO NPs) in anion solutions was inspected in the absence and presence of extracellular polymeric substance (EPS) with a help of time-resolved dynamic light scattering (DLS). The aggregation kinetics and attachment efficiencies were calculated according to measured hydrodynamic diameter across a range of 1-500 mM NaNO and 0.01-100. mM NaSO. The aggregation of CeO NPs in both NaNO and NaSO solution conformed with the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. In NaNO solution, the critical coagulation concentrations (CCC) of CeO NPs was calculated to be about 47 mM; in NaSO solution, CeO NPs showed a re-stabilization process and thus there was no CCC value. SO had intenser effects on CeO NPs aggregation than NO might because of the distinction between their polarization, consisting in Hofmeister series. The presence of bound EPS (B-EPS), tightly bound EPS (TB-EPS) and loosely bound EPS (LB-EPS) in NaNO solutions all lead to significant decrease in CeO NPs aggregation. Steric repulsive force produced by absorbed EPS on CeO NPs might take main responsibility in stabilizing CeO NPs. Besides, Extended Derjaguin-Landau-Verwey-Overbeek (EDLVO) model successfully predicted the energy barrier between CeO NPs with B-EPS, TB-EPS and LB-EPS as a function of NaNO concentration. Furthermore, the difference in impeding the CeO NPs aggregation with B-EPS, TB-EPS and LB-EPS may be caused by the divergence in molecular weight and component mass fraction especially protein content. These results might subserve the assessment on the fate and transport behaviors of CeO NPs released in wastewater treatment plants.

摘要

采用时间分辨动态光散射(DLS)技术,考察了在不存在和存在细胞外聚合物(EPS)的情况下,氧化铈纳米粒子(CeO NPs)在阴离子溶液中的早期聚集情况。根据在 1-500 mM NaNO₃和 0.01-100 mM Na₂SO₄范围内测量的水动力直径,计算了聚集动力学和附着效率。CeO NPs 在 NaNO₃和 Na₂SO₄溶液中的聚集均符合德加古因-朗道-维韦-奥弗贝克(DLVO)理论。在 NaNO₃溶液中,CeO NPs 的临界聚集浓度(CCC)约为 47 mM;在 Na₂SO₄溶液中,CeO NPs 表现出再稳定过程,因此没有 CCC 值。SO 的影响比 NO 更强烈,可能是因为它们的极化作用不同,表现在豪夫迈斯特系列中。在 NaNO₃溶液中存在结合态 EPS(B-EPS)、紧密结合态 EPS(TB-EPS)和松散结合态 EPS(LB-EPS),都会导致 CeO NPs 聚集显著减少。B-EPS 在 CeO NPs 上产生的空间排斥力可能是稳定 CeO NPs 的主要原因。此外,扩展的德加古因-朗道-维韦-奥弗贝克(EDLVO)模型成功预测了 B-EPS、TB-EPS 和 LB-EPS 与 CeO NPs 之间的能量势垒作为 NaNO₃浓度的函数。此外,B-EPS、TB-EPS 和 LB-EPS 阻碍 CeO NPs 聚集的差异可能是由于分子量和成分质量分数(特别是蛋白质含量)的差异造成的。这些结果可能有助于评估污水处理厂中释放的 CeO NPs 的命运和迁移行为。

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