TY - JOUR
T1 - Atmospheric Reactivity of Fullerene (C60) Aerosols
AU - Mitroo, Dhruv
AU - Wu, Jiewei
AU - Colletti, Peter F.
AU - Lee, Seung Soo
AU - Walker, Michael J.
AU - Brune, William H.
AU - Williams, Brent J.
AU - Fortner, John D.
N1 - Funding Information:
National Natural Science Foundation of China (41601228 and 41471194)
Funding Information:
This work was supported by the National Science Foundation Grant 1236865. We would like to thank Adan Montoya, Carl Hinton, and Yining Ou for their help in washing nC60 batches. We would also like to thank Dr. Huafang Li and the Institute of Materials Science & Engineering (IMSE) at Washington University in St. Louis (WUStL) for her valuable assistance and training on the XPS. Finally, we sincerely thank Prof. James Ballard at WUStL and Prof. Dylan Millet at the University of Minnesota (UMN) for insightful discussion and valuable feedback.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2018/2/15
Y1 - 2018/2/15
N2 - 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, nC60 is readily oxidized. This reaction pathway is likely limited by diffusion of oxidants within/through the nC60 aerosol. Further, gas-phase oxidation induces disorder in the crystal structure without affecting aerosol (aggregate) size. Loss of crystallinity suggests aged nC60 aerosols will be less effective ice nuclei, but an increase in surface oxidation will improve their cloud condensation nuclei ability.
AB - 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, nC60 is readily oxidized. This reaction pathway is likely limited by diffusion of oxidants within/through the nC60 aerosol. Further, gas-phase oxidation induces disorder in the crystal structure without affecting aerosol (aggregate) size. Loss of crystallinity suggests aged nC60 aerosols will be less effective ice nuclei, but an increase in surface oxidation will improve their cloud condensation nuclei ability.
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U2 - 10.1021/acsearthspacechem.7b00116
DO - 10.1021/acsearthspacechem.7b00116
M3 - Article
AN - SCOPUS:85043373793
SN - 2472-3452
VL - 2
SP - 95
EP - 102
JO - ACS Earth and Space Chemistry
JF - ACS Earth and Space Chemistry
IS - 2
ER -