Lee Jaesang, Fortner John D, Hughes Joseph B, Kim Jae-Hong
School of Civil and Environmental Engineering, Georgia Institute of Technology, 200 Bobby Dodd Way, Atlanta, Georgia 30332-0373, USA.
Environ Sci Technol. 2007 Apr 1;41(7):2529-35. doi: 10.1021/es062066l.
The objective of this study was to investigate photochemical production of singlet oxygen (1O2) and superoxide radical anion (02*-) by C60 in water. It was demonstrated that photoexcited C60 in the aqueous phase efficiently mediated transfer of absorbed energy to oxygen and produced singlet oxygen when associated with surfactant (Triton X100 and Brij 78) or polymer (polyvinylpyrrolidone), which is consistent with previously observed behavior in organic solvents. However, when C60 was present as colloidal aggregate suspension, prepared through solvent exchange or sonication, this intrinsic character was lost. Similarly, C60 associated with surfactant mediated electron transfer from electron donor (triethylamine) to oxygen producing superoxide radical, while C60 aggregates and C60 associated with polymer did not. These results suggestthat the ability of C60 to mediate energy and electron transfer may be affected by the degree of C60 aggregation in the aqueous phase as well as characteristics of associated stabilizing molecules. Dependence of photochemical reactivity of C60 on its dispersion status in the aqueous phase is critical in assessing environmental impact and cytotoxicity of this material, as C60 associated with model natural organic matter was found to exist in aggregate form and did not produce reactive oxygen species under UV irradiation.
本研究的目的是调查C60在水中光化学生成单线态氧(1O2)和超氧阴离子自由基(02*-)的情况。结果表明,水相中光激发的C60在与表面活性剂(Triton X100和Brij 78)或聚合物(聚乙烯吡咯烷酮)结合时,能有效地将吸收的能量转移给氧气并生成单线态氧,这与之前在有机溶剂中观察到的行为一致。然而,当C60以通过溶剂交换或超声处理制备的胶体聚集体悬浮液形式存在时,这种固有特性就会丧失。同样,与表面活性剂结合的C60介导电子从电子供体(三乙胺)转移到氧气,生成超氧自由基,而C60聚集体和与聚合物结合的C60则不会。这些结果表明,C60介导能量和电子转移的能力可能会受到其在水相中的聚集程度以及相关稳定分子特性的影响。C60的光化学反应性对其在水相中的分散状态的依赖性,对于评估该物质的环境影响和细胞毒性至关重要,因为发现与模型天然有机物结合的C60以聚集形式存在,并且在紫外线照射下不会产生活性氧物种。