Wang Chunyan, Huang Dejuan, He Feiqiang, Jin Tianxiang, Huang Bing, Xu Jianping, Qian Yong
State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang, 330013 Jiangxi, China.
ACS Omega. 2020 Oct 22;5(43):27789-27799. doi: 10.1021/acsomega.0c02715. eCollection 2020 Nov 3.
In the present study, SWCNH-COOH and SWCNH-TETA were fabricated using single-walled carbon nanohorns (SWCNHs) carboxylation and grafting with triethylenetetramine (TETA) for uranium (VI) ion [U(VI)] removal. The morpho-structural characterization of as-prepared adsorbing materials was performed by transmission electron microscopy, X-ray diffractometry, Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). Several parameters including the pH value of the aqueous solutions, contact time, temperature, and U(VI) concentration were used to evaluate the sorption efficiency of SWCNH-COOH and SWCNH-TETA. The Langmuir isotherm model could well represent the as-obtained adsorption isotherms, and the kinetics was successfully modeled by pseudo-second-order kinetics in the adsorption process. The maximum adsorption capacity of SWCNH-TETA was calculated as 333.13 mg/g considering the Langmuir isotherm model. Thermodynamic studies showed that adsorption proved to be a spontaneous endothermic process. Moreover, SWCNH-TETA exhibited excellent recycling performance and selective adsorption of uranium. Furthermore, the possible mechanism was investigated by XPS and density functional theory calculations, indicating that the excellent adsorption was attributed to the cooperation capability between uranium ions and nitrogen atoms in SWCNH-TETA. This efficient approach can provide a strategy for developing high-performance adsorbents for U(VI) removal from wastewater.
在本研究中,通过单壁碳纳米角(SWCNHs)的羧基化以及与三乙烯四胺(TETA)接枝制备了SWCNH - COOH和SWCNH - TETA,用于去除铀(VI)离子[U(VI)]。采用透射电子显微镜、X射线衍射仪、拉曼光谱和X射线光电子能谱(XPS)对所制备的吸附材料进行形态结构表征。使用包括水溶液的pH值、接触时间、温度和U(VI)浓度在内的几个参数来评估SWCNH - COOH和SWCNH - TETA的吸附效率。Langmuir等温线模型能够很好地描述所获得的吸附等温线,并且在吸附过程中动力学成功地用准二级动力学进行了建模。考虑Langmuir等温线模型,计算出SWCNH - TETA的最大吸附容量为333.13 mg/g。热力学研究表明吸附是一个自发的吸热过程。此外,SWCNH - TETA表现出优异的循环性能和对铀的选择性吸附。此外,通过XPS和密度泛函理论计算研究了可能的机理,表明优异的吸附归因于铀离子与SWCNH - TETA中氮原子之间的协同作用能力。这种有效方法可为开发用于从废水中去除U(VI)的高性能吸附剂提供一种策略。