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水流动力学和化学转化控制着银和氧化锌纳米颗粒在流域尺度模型中的环境归宿。

Stream dynamics and chemical transformations control the environmental fate of silver and zinc oxide nanoparticles in a watershed-scale model.

机构信息

†Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.

‡Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States.

出版信息

Environ Sci Technol. 2015 Jun 16;49(12):7285-93. doi: 10.1021/acs.est.5b01205. Epub 2015 Jun 8.

Abstract

Mathematical models are needed to estimate environmental concentrations of engineered nanoparticles (NPs), which enter the environment upon the use and disposal of consumer goods and other products. We present a spatially resolved environmental fate model for the James River Basin, Virginia, that explores the influence of daily variation in streamflow, sediment transport, and stream loads from point and nonpoint sources on water column and sediment concentrations of zinc oxide (ZnO) and silver (Ag) NPs and their reaction byproducts over 20 simulation years. Spatial and temporal variability in sediment transport rates led to high NP transport such that less than 6% of NP-derived metals were retained in the river and sediments. Chemical transformations entirely eliminated ZnO NPs and doubled Zn mobility in the stream relative to Ag. Agricultural runoff accounted for 23% of total metal stream loads from NPs. Average NP-derived metal concentrations in the sediment varied spatially up to 9 orders of magnitude, highlighting the need for high-resolution models. Overall, our results suggest that "first generation" NP risk models have probably misrepresented NP fate in freshwater rivers due to low model resolutions and the simplification of NP chemistry and sediment transport.

摘要

需要数学模型来估计工程纳米颗粒(NPs)的环境浓度,这些颗粒在消费品和其他产品的使用和处置过程中会进入环境。我们提出了一个针对弗吉尼亚州詹姆斯河流域的空间分辨环境归宿模型,该模型探讨了日流量变化、泥沙输运以及点源和非点源对水柱状和沉积物中氧化锌(ZnO)和银(Ag)NPs 及其反应副产物浓度的影响,模拟时间长达 20 年。泥沙输运率的时空变化导致了高 NP 输运,以至于不到 6%的 NP 衍生金属被保留在河流和沉积物中。化学转化完全消除了 ZnO NPs,并使 Ag 相对于 Zn 在溪流中的迁移性增加了一倍。农业径流占 NP 总金属径流量的 23%。沉积物中平均 NP 衍生金属浓度的空间变化高达 9 个数量级,这突出表明需要高分辨率模型。总体而言,我们的研究结果表明,由于模型分辨率低以及 NP 化学和泥沙输运的简化,“第一代”NP 风险模型可能错误地代表了淡水河中的 NP 归宿。

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