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描述在环境相关条件下水中 nC60 的光化学转化特性。

Characterizing photochemical transformation of aqueous nC60 under environmentally relevant conditions.

机构信息

Department of Civil and Environmental Engineering, Rice University, Houston, Texas 77005, USA.

出版信息

Environ Sci Technol. 2010 Apr 15;44(8):3008-13. doi: 10.1021/es903713j.

Abstract

Engineered nanomaterials may undergo transformation upon interactions with various environmental factors. In this study, photochemical transformation of aqueous nC60 was investigated under UVA irradiation. nC60 underwent photochemical transformation in the presence of dissolved O2, resulting in surface oxygenation and hydroxylation as demonstrated by XPS and ATR-FTIR analyses. The reaction followed a pseudo-first order rate law with the apparent reaction rate constant of 2.2 x 10(-2) h(-1). However, the core of the nanoparticles remained intact over 21 days of irradiation. Although no mineralization or dissolution of nC60 was observed, experiments using fullerol as a reference fullerene derivative suggested likely dissolution and partial mineralization of nC60 under long-term UVA exposure. Aquatic humic acid reduced nC60 transformation kinetics presumably due to scavenging of reactive oxygen species. Results from this study imply that photochemical transformation is an important factor controlling nC60 physical and chemical properties as well as its fate and transport in the natural aqueous environment. In addition, changes in nC60 surface chemistry drastically reduced C60 extraction efficiency by toluene, suggesting that the existing analytical method for C60 may not be applicable to environmental samples.

摘要

工程纳米材料在与各种环境因素相互作用时可能会发生转化。在本研究中,研究了在 UVA 照射下水溶液 nC60 的光化学转化。在溶解氧的存在下,nC60 发生光化学转化,XPS 和 ATR-FTIR 分析表明表面发生了氧化和羟化。反应遵循准一级反应定律,表观反应速率常数为 2.2×10^(-2) h^(-1)。然而,在照射 21 天内,纳米颗粒的核心仍然保持完整。尽管没有观察到 nC60 的矿化或溶解,但使用富勒醇作为参考富勒烯衍生物的实验表明,在长期 UVA 暴露下,nC60 可能会溶解和部分矿化。水合腐殖酸降低了 nC60 的转化动力学,可能是由于活性氧物质的清除。本研究的结果表明,光化学转化是控制 nC60 在自然水相环境中的物理化学性质及其归宿和迁移的重要因素。此外,nC60 表面化学的变化极大地降低了甲苯对 C60 的提取效率,表明现有的 C60 分析方法可能不适用于环境样品。

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