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dc.contributor.author Hotze, Ernest M. en_US
dc.contributor.author Wiesner, Mark en_US
dc.date.accessioned 2011-06-21T17:22:07Z
dc.date.available 2011-06-21T17:22:07Z
dc.date.issued 2010 en_US
dc.identifier.citation Hotze,Ernest M.;Bottero,Jean-Yves;Wiesner,Mark R.. 2010. Theoretical Framework for Nanoparticle Reactivity as a Function of Aggregation State. Langmuir 26(13): 11170-11175. en_US
dc.identifier.issn 0743-7463 en_US
dc.identifier.uri http://hdl.handle.net/10161/3994
dc.description.abstract Theory is developed that relates the reactivity of nanoparticles to the structure of aggregates they may form in suspensions. This theory is applied to consider the case of reactive oxygen species (ROS) generation by photosensitization of C-60 fullerenes. Variations in aggregate structure and size appear to account for an apparent paradox in ROS generation as calculated using values for the photochemical kinetics of fullerene (C-60) and its hydroxylated derivative, fullerol (C-60(OH)(22-24)) and assuming that structure varies between compact and fractal objects. A region of aggregation-suppressed ROS production is identified where interactions between the particles in compact aggregates dominate the singlet oxygen production. Intrinsic kinetic properties dominate when aggregates are small and/or are characterized by low fractal dimensions. Pseudoglobal sensitivity analysis of model input variables verifies that fractal dimension, and by extension aggregation state, is the most sensitive model parameter when kinetics are well-known. This theoretical framework qualitatively predicts ROS production by fullerol suspensions 2 orders of magnitude higher compared with aggregates of largely undifferentiated C-60 despite nearly an order of magnitude higher quantum yield for the undifferentiated C-60 based on measurements for single molecules. Similar to C-60, other primary nanoparticles will exist as aggregates in many environmental and laboratory suspensions. This work provides a theoretical basis for understanding how the structure of nanoparticle aggregates may affect their reactivity. en_US
dc.language.iso en_US en_US
dc.publisher AMER CHEMICAL SOC en_US
dc.relation.isversionof doi:10.1021/1a9046963 en_US
dc.subject photophysical properties en_US
dc.subject aqueous-solutions en_US
dc.subject c-60 en_US
dc.subject fullerol en_US
dc.subject water en_US
dc.subject keratinocytes en_US
dc.subject c-60(oh)(18) en_US
dc.subject suspensions en_US
dc.subject mechanisms en_US
dc.subject radiation en_US
dc.subject chemistry, multidisciplinary en_US
dc.subject chemistry, physical en_US
dc.subject materials science, multidisciplinary en_US
dc.title Theoretical Framework for Nanoparticle Reactivity as a Function of Aggregation State en_US
dc.title.alternative en_US
dc.description.version Version of Record en_US
duke.date.pubdate 2010-7-6 en_US
duke.description.endpage 11175 en_US
duke.description.issue 13 en_US
duke.description.startpage 11170 en_US
duke.description.volume 26 en_US
dc.relation.journal Langmuir en_US

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