Yuan Li-Yong, Bai Zhi-Qiang, Zhao Ran, Liu Ya-Lan, Li Zi-Jie, Chu Sheng-Qi, Zheng Li-Rong, Zhang Jing, Zhao Yu-Liang, Chai Zhi-Fang, Shi Wei-Qun
Key Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory for Biomedical Effects of Nanomaterials & Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences , Beijing 100049, China.
ACS Appl Mater Interfaces. 2014 Apr 9;6(7):4786-96. doi: 10.1021/am405584h. Epub 2014 Mar 24.
The potential industrial application of thorium (Th), as well as the environmental and human healthy problems caused by thorium, promotes the development of reliable methods for the separation and removal of Th(IV) from environmental and geological samples. Herein, the phosphonate-amino bifunctionalized mesoporous silica (PAMS) was fabricated by a one-step self-assembly approach for enhancing Th(IV) uptake from aqueous solution. The synthesized sorbent was found to possess ordered mesoporous structures with uniform pore diameter and large surface area, characterized by SEM, XRD, and N2 sorption/desorption measurements. The enhancement of Th(IV) uptake by PAMS was achieved by coupling of an access mechanism to a complexation mechanism, and the sorption can be optimized by adjusting the coverage of the functional groups in the PAMS sorbent. The systemic study on Th(IV) sorption/desorption by using one coverage of PAMS (PAMS12) shows that the Th(IV) sorption by PAMS is fast with equilibrium time of less than 1 h, and the sorption capacity is more than 160 mg/g at a relatively low pH. The sorption isotherm has been successfully modeled by the Langmuir isotherm and D-R isotherm, which reveals a monolayer homogeneous chemisorption of Th(IV) in PAMS. The Th(IV) sorption by PAMS is pH dependent but ionic strength independent. In addition, the sorbed Th(IV) can be completely desorbed using 0.2 mol/L or more concentrated nitric acid solution. The sorption test performed in the solution containing a range of competing metal ions suggests that the PAMS sorbent has a desirable selectivity for Th(IV) ions.
钍(Th)的潜在工业应用以及钍所引发的环境和人类健康问题,推动了从环境和地质样品中分离和去除Th(IV)的可靠方法的发展。在此,通过一步自组装方法制备了膦酸酯-氨基双功能化介孔二氧化硅(PAMS),以增强从水溶液中对Th(IV)的吸附。通过扫描电子显微镜(SEM)、X射线衍射(XRD)和N₂吸附/脱附测量发现,合成的吸附剂具有孔径均匀且比表面积大的有序介孔结构。PAMS对Th(IV)的吸附增强是通过将一种吸附机制与一种络合机制相结合实现的,并且可以通过调整PAMS吸附剂中官能团的覆盖率来优化吸附。使用一种PAMS覆盖率(PAMS12)对Th(IV)吸附/脱附的系统研究表明,PAMS对Th(IV)的吸附很快,平衡时间小于1小时,并且在相对较低的pH值下吸附容量超过160 mg/g。吸附等温线已成功用朗缪尔等温线和D-R等温线进行建模,这表明Th(IV)在PAMS中进行单层均匀化学吸附。PAMS对Th(IV)的吸附取决于pH值,但与离子强度无关。此外,使用0.2 mol/L或更浓的硝酸溶液可以完全解吸吸附的Th(IV)。在含有一系列竞争性金属离子的溶液中进行的吸附测试表明,PAMS吸附剂对Th(IV)离子具有理想的选择性。