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提高富勒烯(nC)聚集体结构的理解:通过静态光散射与非对称流场流分离相结合的分形维数表征。

Improving the understanding of fullerene (nC) aggregate structures: Fractal dimension characterization by static light scattering coupled to asymmetrical flow field flow fractionation.

机构信息

Laboratoire Géosciences Rennes, UMR6118, CNRS/Université de Rennes 1, 263 avenue Général Leclerc, 35000 Rennes, France.

IPREM, UMR 5254 UPPA/CNRS Hélioparc, 2 Avenue du Président Angot, 64053 Pau cedex 09, France.

出版信息

J Colloid Interface Sci. 2017 Sep 15;502:193-200. doi: 10.1016/j.jcis.2017.05.001. Epub 2017 May 3.

Abstract

Fullerene (C) aggregation mechanisms in aqueous media require considerable attention in the near future due to the heavy use and application of fullerene-based products within the context of nanotechnology. Such intensive development will result in the release of massive amounts of C in aqueous environmental systems in the aggregate form (nC). In that sense, the aggregation mechanisms need to be fully determined to better evaluate the environmental fate and behavior of C. To fulfil these needs, the aim of this work was to extensively characterize the aggregation mechanisms of fullerene aggregates in aqueous media by asymmetrical flow field fractionation (AF4) coupled to static light scattering (SLS). We developed a sequential ultrafiltration method that allows the fractionation of the whole nC size distribution into different size classes (1-100-200-450-800nm). Following a preliminary analysis by dynamic light scattering (DLS), we optimized several AF4 separation methods to allow screening of these colloidal size classes of nC with high efficiency and resolution. The fractal dimension (D) of this entire size class was characterized directly on-line according to the radius of gyration through a combination of angle-dependent light scattering and fractal dimension analysis. We demonstrate the possible formation and persistence of colloidal populations of nC in aqueous media from a few nanometers up to 800nm. D values ranging from 1.2 to 2.8, based on the nC colloidal size range, strongly depend on the method of the sample filtration.

摘要

富勒烯(C)在水介质中的聚集机制是未来需要关注的重点,因为在纳米技术的背景下,富勒烯基产品的使用和应用非常广泛。这种密集的开发将导致大量的 C 以聚集形式(nC)释放到水生态系统中。从这个意义上说,需要充分确定聚集机制,以更好地评估 C 的环境归宿和行为。为了满足这些需求,本工作的目的是通过不对称流场分级(AF4)与静态光散射(SLS)相结合,广泛研究富勒烯聚集体在水介质中的聚集机制。我们开发了一种顺序超滤方法,可将整个 nC 粒径分布分级为不同的粒径等级(1-100-200-450-800nm)。通过动态光散射(DLS)进行初步分析后,我们优化了几种 AF4 分离方法,以允许高效和高分辨率地筛选这些胶体粒径等级的 nC。通过结合角度依赖光散射和分形维数分析,根据回转半径直接在线表征整个粒径等级的分形维数(D)。我们证明了在水介质中,从几纳米到 800nm 纳米的 nC 胶体可以形成和稳定存在。基于 nC 胶体粒径范围,D 值从 1.2 到 2.8,强烈依赖于样品过滤的方法。

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