Yang Kun, Wu Wenhao, Jing Qingfeng, Zhu Lizhong
Department of Environmental Science, Zhejiang University, Hangzhou 310028, China.
Environ Sci Technol. 2008 Nov 1;42(21):7931-6. doi: 10.1021/es801463v.
Aqueous adsorption of a series of phenols and anilines by a multiwalled carbon nanotube material (MWCNT15), which depends strongly on the solution pH and the number and types of solute groups, was investigated in this study. The pH-dependent adsorption coefficients, Kd, could be predicted by the established models including solute pKa and solution pH values. Phenol or aniline substitution with more groups has higher adsorption affinity, and nitro, chloride, or methyl groups enhanced adsorption in the following order: nitro group > chloride group > methyl group. All adsorption isotherms of nondissociated phenols and anilines are nonlinear and fitted well bythe Polanyi-theory based Dubinin-Ashtakhov (DA) model. Linear quantitative relationships combining DA model parameters (E and b) with solute solvatochromic parameters were developed to evaluate the adsorptive behaviors of nondissociated species. For the saturated sorbed capacity, Q0, the logarithmic values of phenols and anilines were relatively constant with a mean value of 1.90. Besides the van der Waals force, H-bonding interactions from solutes as hydrogen-bonding donors, and followed by pi-electron polarizability, may play important roles on the adsorption of phenols and anilines by carbon nanotubes in the aqueous environment
本研究考察了多壁碳纳米管材料(MWCNT15)对一系列酚类和苯胺类物质的水相吸附情况,其吸附作用强烈依赖于溶液pH值以及溶质基团的数量和类型。pH依赖的吸附系数Kd可以通过包括溶质pKa和溶液pH值在内的已建立模型进行预测。具有更多基团的酚或苯胺取代物具有更高的吸附亲和力,硝基、氯或甲基对吸附的增强作用顺序如下:硝基>氯基团>甲基基团。所有未解离酚类和苯胺类物质的吸附等温线均为非线性,并且能很好地用基于Polanyi理论的Dubinin-Ashtakhov(DA)模型拟合。建立了将DA模型参数(E和b)与溶质溶剂化显色参数相结合的线性定量关系,以评估未解离物质的吸附行为。对于饱和吸附容量Q0,酚类和苯胺类物质的对数值相对恒定,平均值为1.90。除范德华力外,溶质作为氢键供体的氢键相互作用,以及随后的π电子极化率,可能在水环境中碳纳米管对酚类和苯胺类物质的吸附中起重要作用