State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
Environ Sci Pollut Res Int. 2014 Mar;21(6):4358-65. doi: 10.1007/s11356-013-2304-7. Epub 2013 Dec 10.
Surface oxygen functional groups can affect the morphological characteristics, aggregation kinetics, and adsorption capacity of multi-walled carbon nanotubes (MWCNTs). However, little is known about the quantitative relationship between oxygen content and the dispersion stability of MWCNTs. To investigate the effects of surface oxidization, MWCNTs were oxidized using concentrated H2SO4/HNO3 acids for 0, 1, 2, 4, and 8 h, respectively. Experimental results showed that the oxygen content of MWCNTs increased with surface oxidization time. Linear correlations were found to exist between the oxygen content, critical coagulation concentration (CCC) for NaCl, and critical coagulation pH values of MWCNTs detected by optical density at 800 nm. The CCC values for CaCl2 increased with oxygen contents for unmodified MWCNTs and lowly oxidized MWCNTs, while which decreased after further increasing the surface oxidization. CCC ratios in the presence of Ca(2+) to Na(+) were consistent with the empirical Schulze-Hardy rule for unmodified MWCNTs and lowly oxidized MWCNTs; however, which were much lower than the expected values for highly oxidized MWCNTs. Fulvic acid can clearly increase the stability of MWCNT suspension with unmodified MWCNTs and lowly oxidized MWCNTs, while it cannot affect the dispersion of highly oxidized MWCNTs. This study implied that the oxidation and presence of fulvic acid will possibly increase the mobility, exposure, bioavailability, and toxicity of MWCNTs.
表面氧官能团会影响多壁碳纳米管(MWCNTs)的形态特征、聚集动力学和吸附能力。然而,对于氧含量与 MWCNTs 分散稳定性之间的定量关系知之甚少。为了研究表面氧化的影响,MWCNTs 分别用浓 H2SO4/HNO3 酸氧化 0、1、2、4 和 8 h。实验结果表明,MWCNTs 的氧含量随表面氧化时间的增加而增加。通过 800nm 处光密度检测到的 MWCNTs 的氧含量、NaCl 的临界聚沉浓度(CCC)和临界聚沉 pH 值之间存在线性关系。对于未改性 MWCNTs 和低氧化 MWCNTs,CCC 值随氧含量的增加而增加,而在进一步增加表面氧化后则降低。在存在 Ca(2+)和 Na(+)的情况下,CCC 比值与未改性 MWCNTs 和低氧化 MWCNTs 的经验 Schulze-Hardy 规则一致;然而,对于高度氧化的 MWCNTs,其值远低于预期值。富里酸可以明显增加未改性 MWCNTs 和低氧化 MWCNTs 悬浮液的稳定性,而对高度氧化 MWCNTs 的分散性没有影响。这项研究表明,氧化和富里酸的存在可能会增加 MWCNTs 的迁移性、暴露度、生物利用度和毒性。