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pH值和磷酸盐对二氧化铈纳米颗粒溶解的影响。

Effects of pH and phosphate on CeO2 nanoparticle dissolution.

作者信息

Dahle Jessica T, Livi Ken, Arai Yuji

机构信息

Clemson University, School of Agricultural, Forest and Environmental Sci., Clemson, SC 29634, USA.

The Integrated Imaging Center/HRAEM Facility, Departments of Earth and Planetary Sci., Johns Hopkins University, Baltimore, MD 21218, USA.

出版信息

Chemosphere. 2015 Jan;119:1365-1371. doi: 10.1016/j.chemosphere.2014.02.027. Epub 2014 Mar 12.

Abstract

As the result of rapidly grown nanotechnology industries, release of engineered nanoparticles (ENPs) to environment has increased, posing in a serious risk to environmental and human health. To better understand the chemical fate of ENPs in aquatic environments, solubility of CeO2 NPs was investigated using batch dissolution experiments as a function of pH (1.65-12.5), [phosphate] and particle size (33 and 78 nm). It was found that CeO2 dissolution was only significant at pH<5 and inversely proportional to surface area. After 120 h, the release of Ce was ∼3 times greater in large NPs than that in small NPs that is likely contributed by the difference in exchangeable Ce(III) impurity (small: 0.3 mM kg(-1), large: 1.56 mM kg(-1)). When 100 μM of phosphate was added, the dissolution rate of CeO2 NPs was decreased in small NPs by 15% at pH 1.65 and 75% at pH 4.5 and in large NPs by 56% at pH 1.65 and 63% at pH 4.5. The inner-sphere surface complexation of P that is revealed by the zeta potential measurements is effectively suppressing the CeO2 NP dissolution. Predicting the fate and transport of CeO2 NPs in aquatic environment, pH and P ligands might play important roles in controlling the solubility of CeO2 NPs.

摘要

随着纳米技术产业的迅速发展,工程纳米颗粒(ENPs)向环境中的释放量增加,对环境和人类健康构成严重风险。为了更好地了解ENPs在水生环境中的化学归宿,通过批次溶解实验研究了CeO2纳米颗粒的溶解度与pH值(1.65 - 12.5)、[磷酸盐]和粒径(33和78纳米)的关系。结果发现,CeO2的溶解仅在pH<5时显著,且与表面积成反比。120小时后,大尺寸纳米颗粒中Ce的释放量比小尺寸纳米颗粒中约大3倍,这可能是由于可交换Ce(III)杂质的差异造成的(小尺寸:0.3 mM kg(-1),大尺寸:1.56 mM kg(-1))。当添加100 μM磷酸盐时,在pH 1.65时小尺寸纳米颗粒中CeO2纳米颗粒的溶解速率降低了15%,在pH 4.5时降低了75%;在pH 1.65时大尺寸纳米颗粒中降低了56%,在pH 4.5时降低了63%。ζ电位测量揭示的P的内球表面络合有效地抑制了CeO2纳米颗粒的溶解。预测CeO2纳米颗粒在水生环境中的归宿和迁移,pH值和P配体可能在控制CeO2纳米颗粒的溶解度方面发挥重要作用。

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