Dahle Jessica T, Livi Ken, Arai Yuji
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.
Chemosphere. 2015 Jan;119:1365-1371. doi: 10.1016/j.chemosphere.2014.02.027. Epub 2014 Mar 12.
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.
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。