Photochemical and Photophysical Properties of Sequentially Functionalized Fullerenes in the Aqueous Phase
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- 作者：Samuel D. Snow ; Jaesang Lee ; Jae-Hong Kim
- 刊名：Environmental Science & Technology (ES&T)
- 出版年：2012
- 出版时间：December 18, 2012
- 年：2012
- 卷：46
- 期：24
- 页码：13227-13234
- 全文大小：427K
- 年卷期：v.46,no.24(December 18, 2012)
- ISSN：1520-5851
文摘
The vast range of C60 derivatives makes it difficult to assess the potential environmental impact of this class of materials, while past environmental studies mostly focused only on pristine C60. Central to derivatized C60鈥檚 potential to negatively impact (micro)biological receptors upon unintended release is its unique property of mediating the transfer of light energy to ambient oxygen, producing 1O2. To initiate the process of establishing a thorough understanding of the photoinduced adverse biological effects of functionalized fullerenes and their aqueous dispersions, the photochemical properties relevant to 1O2 production were evaluated using three selected series of mono-, bis-, and tris-adducted fullerene materials. Differential 1O2 production of derivatives in toluene were explained by spectral variations under visible and UVA light conditions. Of the nine functionalities studied only aggregates of two positively charged derivatives showed significant photoactivity under experimental conditions. Laser flash photolysis revealed a triplet excited state in the photoactive aggregates with a sufficiently long lifetime to be quenched by 3O2. Dynamic light scattering, transmission electron microscopy, and electron diffraction patterns revealed aggregates with sizes typical of aqueous C60 colloids that varied in crystallinity based on functionality. Results raised questions about our current understanding of the photoactivity of fullerene aggregates.