How Redox Conditions and Irradiation Affect Sorption of PAHs by Dispersed Fullerenes (nC60)

Thorsten Hüffer; Melanie Kah; Thilo Hofmann; Torsten C. Schmidt

doi:10.1021/es303620c

How Redox Conditions and Irradiation Affect Sorption of PAHs by Dispersed Fullerenes (nC60)

Thorsten Hüffer
, Melanie Kah
, Thilo Hofmann (Corresponding author)
, Torsten C. Schmidt (Corresponding author)

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

Surface properties, dispersion state, and sorption behavior of carbon-based nanomaterials will change after being released into the environment. To study these processes, five different scenarios were considered to probe the impact of changes in surface properties of dispersed fullerenes (nC60) on their sorption potential due to irradiation and presence of oxygen. Sorption isotherms of pyrene by nC60 were determined at environmentally relevant concentrations applying a passive sampling method. Isotherms of all dispersion scenarios were best fit with the Dubinin-Ashthakov model. Sorption was strongest for nC60 kept under anoxic condition. Both the presence of oxygen and irradiation significantly decreased the sorption capacity of nC60, while commercially available polyhydroxy fullerenes had the smallest sorption. In addition, competition for sorption sites was never observed in multiple sorbate experiments with four polycyclic aromatic hydrocarbons at small concentration. A strong relationship between sorption coefficients and hydrophobic properties of sorbates suggests that hydrophobic interactions are of major importance. The results emphasize that aging of released fullerenes results in a reduced strength of interactions with nonpolar compounds and, thus, reduces the impact on the environmental transport of hydrophobic pollutants

Original language	English
Pages (from-to)	6935-6942
Number of pages	8
Journal	Environmental Science & Technology
Volume	47
Issue number	13
DOIs	https://doi.org/10.1021/es303620c
Publication status	Published - 2 Jul 2013

Funding

We thank Petra Korner for her assistance in the laboratory, Samuel Legros for his support with the DLS measurements, Kristina Straub for preparing anoxic background solutions (Department of Environmental Geosciences, University of Vienna), and Felix Becker (Department of Physics, University of Duisburg-Essen) for the XPS data. The comments by three anonymous reviewers significantly improved our manuscript. This work was partly financed by the German Research Foundation (SCHM 1372/10-1).

Austrian Fields of Science 2012

210006 Nanotechnology
104002 Analytical chemistry
104023 Environmental chemistry
105904 Environmental research

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10.1021/es303620c

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title = "How Redox Conditions and Irradiation Affect Sorption of PAHs by Dispersed Fullerenes (nC60)",

abstract = "Surface properties, dispersion state, and sorption behavior of carbon-based nanomaterials will change after being released into the environment. To study these processes, five different scenarios were considered to probe the impact of changes in surface properties of dispersed fullerenes (nC60) on their sorption potential due to irradiation and presence of oxygen. Sorption isotherms of pyrene by nC60 were determined at environmentally relevant concentrations applying a passive sampling method. Isotherms of all dispersion scenarios were best fit with the Dubinin-Ashthakov model. Sorption was strongest for nC60 kept under anoxic condition. Both the presence of oxygen and irradiation significantly decreased the sorption capacity of nC60, while commercially available polyhydroxy fullerenes had the smallest sorption. In addition, competition for sorption sites was never observed in multiple sorbate experiments with four polycyclic aromatic hydrocarbons at small concentration. A strong relationship between sorption coefficients and hydrophobic properties of sorbates suggests that hydrophobic interactions are of major importance. The results emphasize that aging of released fullerenes results in a reduced strength of interactions with nonpolar compounds and, thus, reduces the impact on the environmental transport of hydrophobic pollutants",

author = "Thorsten H{\"u}ffer and Melanie Kah and Thilo Hofmann and Schmidt, \{Torsten C.\}",

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AU - Hüffer, Thorsten

AU - Kah, Melanie

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AU - Schmidt, Torsten C.

PY - 2013/7/2

Y1 - 2013/7/2

N2 - Surface properties, dispersion state, and sorption behavior of carbon-based nanomaterials will change after being released into the environment. To study these processes, five different scenarios were considered to probe the impact of changes in surface properties of dispersed fullerenes (nC60) on their sorption potential due to irradiation and presence of oxygen. Sorption isotherms of pyrene by nC60 were determined at environmentally relevant concentrations applying a passive sampling method. Isotherms of all dispersion scenarios were best fit with the Dubinin-Ashthakov model. Sorption was strongest for nC60 kept under anoxic condition. Both the presence of oxygen and irradiation significantly decreased the sorption capacity of nC60, while commercially available polyhydroxy fullerenes had the smallest sorption. In addition, competition for sorption sites was never observed in multiple sorbate experiments with four polycyclic aromatic hydrocarbons at small concentration. A strong relationship between sorption coefficients and hydrophobic properties of sorbates suggests that hydrophobic interactions are of major importance. The results emphasize that aging of released fullerenes results in a reduced strength of interactions with nonpolar compounds and, thus, reduces the impact on the environmental transport of hydrophobic pollutants

AB - Surface properties, dispersion state, and sorption behavior of carbon-based nanomaterials will change after being released into the environment. To study these processes, five different scenarios were considered to probe the impact of changes in surface properties of dispersed fullerenes (nC60) on their sorption potential due to irradiation and presence of oxygen. Sorption isotherms of pyrene by nC60 were determined at environmentally relevant concentrations applying a passive sampling method. Isotherms of all dispersion scenarios were best fit with the Dubinin-Ashthakov model. Sorption was strongest for nC60 kept under anoxic condition. Both the presence of oxygen and irradiation significantly decreased the sorption capacity of nC60, while commercially available polyhydroxy fullerenes had the smallest sorption. In addition, competition for sorption sites was never observed in multiple sorbate experiments with four polycyclic aromatic hydrocarbons at small concentration. A strong relationship between sorption coefficients and hydrophobic properties of sorbates suggests that hydrophobic interactions are of major importance. The results emphasize that aging of released fullerenes results in a reduced strength of interactions with nonpolar compounds and, thus, reduces the impact on the environmental transport of hydrophobic pollutants

U2 - 10.1021/es303620c

DO - 10.1021/es303620c

M3 - Article

SN - 0013-936X

VL - 47

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JO - Environmental Science & Technology

JF - Environmental Science & Technology

IS - 13

ER -

How Redox Conditions and Irradiation Affect Sorption of PAHs by Dispersed Fullerenes (nC60)

Abstract

Funding

Austrian Fields of Science 2012

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