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In Situ Observations of Nanoparticle Early Development Kinetics at Mineral-Water Interfaces

机译：矿泉水界面纳米颗粒早期发育动力学的原位观察

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摘要

The early development of nanoparticles at mineral-water interfaces exerts crucial influences on the sequestration and transport of aqueous toxic species originating from both natural and anthropogenic sources. Homogeneous and heterogeneous nucleation often occur simultaneously, making it difficult to sort out whether toxic species are transported as free species, sorbed on nanoparticle surfaces, or trapped between aggregated nanoparticles. Here, using a newly developed X-ray scattering setup, we show how homogeneous nucleation and growth can be quantitatively separated from heterogeneous processes under aqueous conditions in real-time. Under conditions found in acid-mine-drainage (at pH 3.6 and [Fe~(3+)] = 10~(-4)M), heterogeneous nucleation of iron oxide nanoparticles on quartz dominated homogeneous nucleation by a factor of 192 (by particle volume). The smallest heterogeneously formed nanoparticles had radii of 1.7 ± 0.5 nm, significantly smaller than the size estimated using classical nucleation theory (CNT). Based on the data, the dominant nucleation and growth mechanisms of iron oxide nanoparticles depending on ionic strength were presented. Our findings have implications for the formation and transport of nanoparticles, and thus toxins, in both environmental and biological systems.
机译：矿物质-水界面处纳米粒子的早期发展对源自自然和人为来源的水性有毒物质的隔离和运输产生了至关重要的影响。均相和异相成核通常同时发生，这使得很难区分有毒物质是作为自由物质运输，被吸附在纳米颗粒表面还是被聚集在纳米颗粒之间。在这里，使用最新开发的X射线散射装置，我们展示了如何在水性条件下实时地将均相成核和生长与异质过程定量分离。在排酸的条件下（在pH 3.6且[Fe〜（3+）] = 10〜（-4）M）下，氧化铁纳米颗粒在石英上的异质成核作用是均匀成核作用的192倍（通过颗粒体积）。最小的异质形成纳米颗粒的半径为1.7±0.5 nm，大大小于使用经典成核理论（CNT）估计的尺寸。基于这些数据，提出了取决于离子强度的氧化铁纳米粒子的主要成核和生长机理。我们的发现对环境和生物系统中纳米颗粒的形成和运输以及毒素产生了影响。

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  • 来源
    《Environmental Science & Technology》 |2010年第21期|p.8182-8189|共8页
  • 作者

    YOUNG-SHIN JUN; BYEONGDU LEE; GLENN A. WAYCHUNAS;

  • 作者单位

    Department of Energy, Environmental and Chemical Engineering, Washington University, St. Louis, Missouri 63130, United States;

    rnX-ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States;

    rnEarth Science Division, Geochemistry Department, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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