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富勒烯在水溶液中的聚集行为:毛细管电泳和不对称流场-流分馏研究

Aggregation behavior of fullerenes in aqueous solutions: a capillary electrophoresis and asymmetric flow field-flow fractionation study.

作者信息

Astefanei Alina, Núñez Oscar, Galceran Maria Teresa, Kok Wim Th, Schoenmakers Peter J

机构信息

Department of Analytical Chemistry, University of Barcelona, Martí i Franquès 1-11, 08028, Barcelona, Spain.

Serra Húnter Fellow, Generalitat de Catalunya, Barcelona, Spain.

出版信息

Anal Bioanal Chem. 2015 Oct;407(26):8035-45. doi: 10.1007/s00216-015-8976-8. Epub 2015 Aug 28.

Abstract

In this work, the electrophoretic behavior of hydrophobic fullerenes [buckminsterfullerene (C60), C70, and N-methyl-fulleropyrrolidine (C60-pyrr)] and water-soluble fullerenes [fullerol (C60(OH)24); polyhydroxy small gap fullerene, hydrated (C120(OH)30); C60 pyrrolidine tris acid (C60-pyrr tris acid); and (1,2-methanofullerene C60)-61-carboxylic acid (C60CHCOOH)] in micellar electrokinetic capillary chromatography (MECC) was evaluated. The aggregation behavior of the water-soluble compounds in MECC at different buffer and sodium dodecyl sulfate (SDS) concentrations and pH values of the background electrolyte (BGE) was studied by monitoring the changes observed in the electrophoretic pattern of the peaks. Broad and distorted peaks that can be attributed to fullerene aggregation were obtained in MECC which became narrower and more symmetric by working at low buffer and SDS concentrations (below the critical micelle concentration, capillary zone electrophoresis (CZE) conditions). For the characterization of the suspected aggregates formed (size and shape), asymmetrical flow field-flow fractionation (AF4) and transmission electron microscopy (TEM) were used. The results showed that the increase in the buffer concentration promoted the aggregation of the particles, while the presence of SDS micelles revealed multiple peaks corresponding to particles of different aggregation degrees. Furthermore, MECC has been applied for the first time for the analysis of C60 in two different cosmetic products (i.e., anti-aging serum and facial mask).

摘要

在本研究中,评估了疏水性富勒烯[巴克敏斯特富勒烯(C60)、C70和N-甲基-富勒吡咯烷(C60-吡咯)]以及水溶性富勒烯[富勒醇(C60(OH)24);多羟基小间隙富勒烯,水合(C120(OH)30);C60吡咯烷三酸(C60-吡咯三酸);以及(1,2-亚甲基富勒烯C60)-61-羧酸(C60CHCOOH)]在胶束电动毛细管色谱(MECC)中的电泳行为。通过监测峰的电泳图谱中观察到的变化,研究了水溶性化合物在MECC中于不同缓冲液、十二烷基硫酸钠(SDS)浓度以及背景电解质(BGE)的pH值下的聚集行为。在MECC中获得了可归因于富勒烯聚集的宽峰和变形峰,通过在低缓冲液和SDS浓度(低于临界胶束浓度,毛细管区带电泳(CZE)条件)下工作,这些峰变得更窄且更对称。为了表征形成所怀疑的聚集体(尺寸和形状),使用了不对称流场-流分级(AF4)和透射电子显微镜(TEM)。结果表明,缓冲液浓度的增加促进了颗粒的聚集,而SDS胶束的存在揭示了对应于不同聚集程度颗粒的多个峰。此外,MECC首次被应用于分析两种不同化妆品(即抗衰血清和面膜)中的C60。

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