National Exposure Research Laboratory, Office of Research and Development, U.S. EPA, Athens, Georgia, USA.
Environ Sci Technol. 2011 Jun 15;45(12):5170-7. doi: 10.1021/es1041145. Epub 2011 May 17.
Little is known about how temporal changes in the physical-chemical properties of C₆₀ aggregates formed in aqueous systems (termed aqu/C₆₀) can impact transport pathways contributing to ecological exposures. In this study three aqu/C₆₀ suspensions of short-term (100 days), intermediate-term (300 days), and long-term (1000 days) water exposure were first characterized for particle size distribution, water/toluene phase distribution, and surface chemistry. Then, aqu/C₆₀ deposition to a model silica surface and transport in porous media were studied by quartz crystal microbalance (QCM) and saturated sand columns. As suspension time increased, aqu/C₆₀ particle size shifted to a larger size range as determined by asymmetric flow field-flow fractionation (AF4) and the aqu/C₆₀ distribution to toluene was reduced, likely due to surface polarization as revealed by nuclear magnetic resonance (NMR) and UV-visible spectroscopy of the aqu/C₆₀ suspensions. Additionally, the deposition to silica surfaces in both QCM and column studies decreased with increased water exposure time. Although a small increase in aqu/C₆₀ aggregate size with time may partially explain the greater transport of the long-term aqu/C₆₀ because of the decreased collector efficiency for larger submicrometer particles, the polarization of the aqu/C₆₀ (thus a more hydrophilic surface) revealed by the toluene/water phase distribution and confirmed by NMR, is considered the determining factor.
关于在水系统中形成的 C₆₀ 聚集体的物理化学性质随时间的变化如何影响导致生态暴露的传输途径,人们知之甚少。在这项研究中,首先对三种短期(100 天)、中期(300 天)和长期(1000 天)水暴露的 aqu/C₆₀ 悬浮液进行了粒径分布、水/甲苯相分布和表面化学特性的表征。然后,通过石英晶体微天平(QCM)和饱和砂柱研究了 aqu/C₆₀ 在模型硅表面上的沉积和在多孔介质中的传输。随着悬浮时间的增加,如通过不对称流场流分离(AF4)确定的 aqu/C₆₀ 粒径向较大的粒径范围转移,以及 aqu/C₆₀ 向甲苯的分配减少,可能是由于 NMR 和 aqu/C₆₀ 悬浮液的紫外-可见光谱揭示的表面极化所致。此外,在 QCM 和柱研究中,水暴露时间增加导致 aqu/C₆₀ 在硅表面上的沉积减少。尽管随着时间的推移,aqu/C₆₀ 聚集体的尺寸略有增加,可能部分解释了长期 aqu/C₆₀ 传输的增加,因为较大的亚微米颗粒的收集效率降低,但甲苯/水相分布和 NMR 证实的 aqu/C₆₀ 的极化(因此更亲水的表面)被认为是决定性因素。