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在模拟环境相关条件下的紫外光照射下对固态 C60 富勒烯进行孵化。

Incubation of solid state C fullerene under UV irradiation mimicking environmentally relevant conditions.

机构信息

University of Amsterdam, Institute for Biodiversity and Ecosystem Dynamics, Science Park 904, 1098 XH Amsterdam, The Netherlands.

University of Amsterdam, Institute for Biodiversity and Ecosystem Dynamics, Science Park 904, 1098 XH Amsterdam, The Netherlands.

出版信息

Chemosphere. 2017 May;175:1-7. doi: 10.1016/j.chemosphere.2017.01.149. Epub 2017 Feb 2.

DOI:10.1016/j.chemosphere.2017.01.149
PMID:28211322
Abstract

Carbon-based nanomaterials, such as C fullerenes, are expected to accumulate in soil due to direct release and deposition from the atmosphere. However, little is known about the environmental fate of these nanoparticles which may be susceptible to photochemical and microbial degradation. In the present work, C was incubated for a period of 28 days and irradiated with UVA light. Three experiments were carried out where the fullerenes were either spiked onto a glass surface or added to quartz sand or sandy soil samples. At specific time intervals the samples were extracted and analysed by liquid chromatography coupled to UV or high resolution mass spectrometric (HRMS) detection. The fullerenes were degraded in all the treatments and the decay followed a pseudo-first-order rate law. In absence of a solid matrix, the half-life (t) of the C was 13.1 days, with an overall degradation of 45.1% that was accompanied by the formation of functionalized C-like structures. Furthermore, mass spectrometric analysis highlighted the presence of a large number of transformation products that were not directly related to the irradiation and presented opened cage and oxidized structures. When C was spiked into solid matrices the degradation occurred at a faster rate (t of 4.5 and 0.8 days for quartz sand and sandy soil, respectively). Minor but consistent losses were found in the non-irradiated samples, presumably due to biotic or chemical processes occurring in these samples. The results of this study suggest that light-mediated transformation of the fullerenes will occur in the environment.

摘要

碳基纳米材料,如 C60 富勒烯,预计会由于直接释放和大气沉降而在土壤中积累。然而,对于这些纳米颗粒的环境归宿,人们知之甚少,它们可能容易受到光化学和微生物降解的影响。在本工作中,C60 被孵育了 28 天,并接受了 UVA 光的辐照。进行了三个实验,其中富勒烯要么被喷洒在玻璃表面上,要么添加到石英砂或沙土样品中。在特定的时间间隔内,提取并通过液相色谱法与紫外或高分辨率质谱(HRMS)检测进行分析。在所有处理中,富勒烯都被降解了,衰减遵循拟一级动力学规律。在没有固体基质的情况下,C60 的半衰期(t)为 13.1 天,整体降解率为 45.1%,同时伴随着官能化的 C 样结构的形成。此外,质谱分析突出了大量与辐照无关的转化产物的存在,这些产物呈现出开笼和氧化结构。当 C60 被喷洒到固体基质中时,降解发生得更快(在石英砂和沙土中的半衰期分别为 4.5 和 0.8 天)。在未辐照的样品中也发现了少量但一致的损失,这可能是由于这些样品中发生了生物或化学过程。本研究的结果表明,富勒烯的光介导转化将在环境中发生。

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