Atmospheric Reactivity of Fullerene (C 60 ) Aerosols

Atmospheric Reactivity of Fullerene (C 60 ) Aerosols
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富勒烯 (C 60 ) 气溶胶的大气反应性

DOI:
10.1021/acsearthspacechem.7b00116
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发表时间:
2018
影响因子:
3.4
通讯作者:
Fortner, John D.
Fortner, John D.
中科院分区:
化学3区
文献类型:
--
作者:
Mitroo, Dhruv;Wu, Jiewei;Colletti, Peter F.;Lee, Seung Soo;Walker, Michael J.;Brune, William H.;Williams, Brent J.;Fortner, John D.

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以纳米材料为基础的技术的快速增长和采用,为不明材料向环境释放的风险奠定了基础。碳基材料,特别是富勒烯,已被广泛提出用于各种应用。对它们行为的定量了解对于准确的环境影响评估是至关重要的。虽然它们的水相反应性、去向和传输已经被研究了十多年,但气溶胶相的反应性仍然没有被探索。在这里,作为纳米晶(NC60)气溶胶的C60的转变是在一系列模拟大气条件下评估的。在紫外光、气相臭氧和·OH的照射下,nC60很容易被氧化。这一反应途径可能受到氧化剂在C60气溶胶内/通过C60气溶胶扩散的限制。此外,气相氧化在不影响气溶胶(聚集体)大小的情况下导致晶体结构的无序。结晶度的丧失表明,老化的C60气溶胶将不是有效的冰核,但表面氧化的增加将改善它们的云凝聚核能力。
Rapid growth and adoption of nanomaterial-based technologies underpin a risk for unaccounted material release to the environment. Carbon-based materials, in particular fullerenes, have been widely proposed for a variety of applications. A quantitative understanding of how they behave is critical for accurate environmental impact assessment. While their aqueous phase reactivity, fate, and transport have been studied for over a decade, aerosol phase reactivity remains unexplored. Here, the transformation of C60, as nanocrystal (nC60) aerosols, is evaluated over a range of simulated atmospheric conditions. Upon exposure to UV light, gas-phase O3, and•OH,nC60is readily oxidized. This reaction pathway is likely limited by diffusion of oxidants within/through thenC60aerosol. Further, gas-phase oxidation induces disorder in the crystal structure without affecting aerosol (aggregate) size. Loss of crystallinity suggests agednC60aerosols will be less effective ice nuclei, but an increase in surface oxidation will improve their cloud condensation nuclei ability.