State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, China.
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, China.
Sci Total Environ. 2014 Sep 15;493:12-21. doi: 10.1016/j.scitotenv.2014.05.107. Epub 2014 Jun 14.
The wide application of engineered carbon nanomaterials, such as fullerene (C60), will inevitably result in their introduction into the aqueous environment. Interactions of C60 with abundant natural organic matter (NOM) will likely alter the bioavailability of organic compounds to aquatic organisms. The availability of 12 types of polycyclic aromatic hydrocarbons (PAHs) in various aqueous suspensions of fullerene (nC60) prepared by different methods, e.g., in humic acid (HA) and particularly in combined systems of nC(60) and HA, was investigated by negligible depletion solid-phase microextraction (nd-SPME). The results showed that HA accelerated the rate constants (k2) of almost all PAH uptakes to the nd-SPME fibers compared with the solutions without the matrix; the combined matrices of nC(60) and HA significantly promoted the k2 of highly hydrophobic PAHs (logKOW 5.81-6.20), whereas they retarded that of less hydrophobic ones (logKOW 3.82-4.63) (p<0.05). Remarkable or minor reduction of free concentration of PAH was observed in the combined system of nC(60) and HA depending on the properties of individual PAHs. Sorption coefficients (KHA, K(C60) and K(C60+HA)) of various PAHs in different matrices were provided, and matrix concentrations showed no significant effects. For highly hydrophobic PAHs (logKOW 5.16-6.20), the logK(C60+HA) >= logKHA > logK(C60), whereas for less hydrophobic PAHs (logKOW 3.8-4.63), the Kmatrix values in various matrices showed no noticeable trend. In addition, higher K(C60) values were obtained for aqu/nC(60) than for son/nC(60) for most highly hydrophobic PAHs. The above results suggest that hydrophobicity plays an important role in determining Kmatrix in addition to the matrix effects. The interactions between nC(60) and HA have critical or minor impacts on availability, and thus bioavailability, of PAHs. This paper contributes to the understanding of the bioavailability mechanisms of organic pollutants in the aquatic environment with both nC(60) and NOM.
工程碳纳米材料（如富勒烯（C60））的广泛应用将不可避免地导致其进入水环境。C60 与丰富的天然有机物（NOM）的相互作用可能会改变有机化合物对水生生物的生物利用度。通过可忽略的消耗固相微萃取（nd-SPME）研究了通过不同方法制备的富勒烯（nC60）在各种水溶液悬浮液中的 12 种多环芳烃（PAHs）的可用性，例如在腐殖酸（HA）中，特别是在 nC（60）和 HA 的组合系统中。结果表明，与没有基质的溶液相比，HA 加速了几乎所有 PAH 被 nd-SPME 纤维吸收的速率常数（k2）; nC（60）和 HA 的组合基质显著促进了高疏水性 PAHs（logKOW 5.81-6.20）的 k2，而它们则延迟了疏水性较小的 PAHs（logKOW 3.82-4.63）的 k2（p<0.05）。在 nC（60）和 HA 的组合系统中观察到 PAH 的游离浓度有显著或轻微降低，这取决于各个 PAH 的性质。提供了各种 PAH 在不同基质中的分配系数（KHA、K（C60）和 K（C60+HA）），并且基质浓度没有显示出明显的影响。对于高疏水性 PAHs（logKOW 5.16-6.20），logK（C60+HA）>=logKHA>logK（C60），而对于疏水性较小的 PAHs（logKOW 3.8-4.63），各种基质中的 Kmatrix 值没有明显的趋势。此外，对于大多数高疏水性 PAHs，水相/nC（60）的 K（C60）值高于超声/nC（60）的 K（C60）值。上述结果表明，疏水性除了基质效应外，在确定 Kmatrix 方面起着重要作用。nC（60）和 HA 之间的相互作用对 PAHs 的可用性以及因此对生物利用度具有关键或轻微的影响。本文有助于理解含有 nC（60）和 NOM 的水环境污染中有机污染物的生物利用机制。
