School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China.
School of Chemistry and Biology Engineering, University of Science and Technology Beijing, 100083 Beijing, China.
J Hazard Mater. 2022 Jul 5;433:128728. doi: 10.1016/j.jhazmat.2022.128728. Epub 2022 Mar 29.
Technetium-99 (Tc) is a long-lived radioactive nuclide that poses great threat to environment, hence selective removal of Tc from aquatic system is always an issue. Aminomethylpyridine (AMP) equipped with pyridine and amino, is a promising receptor for TcO and its surrogate ReO, thus it is of interest to explore and understand the structure-properties relationship of ReO adsorption related to n-AMP structure that differ in amino methyl position. In this work, three n-AMP functionalized cellulose microspheres (n-AMPR, n = 2, 3, 4) were synthesized and employed for TcO/ReO uptake. The effect of aminomethyl position on adsorption properties of n-AMPR for ReO were investigated and compared. Adsorption kinetics and adsorption isotherm showed that adsorption speed and adsorption capacity were in order of 3-AMPR > 2-AMPR > 4-AMPR. DFT calculation verified that the adsorption of ReO by n-AMPR was attributed to electrostatic interaction and hydrogen bonding interaction, the order of adsorption abilities of n-AMPR was due to that steric effect and hydrogen bond collaborated in stabilizing n-AMPR-ReO complexes. The column experiments demonstrated that 3-AMPR can be selectively remove ReO from simulated groundwater. More importantly, Tc column experiments showed that 3-AMPR had a better ability for actual radioactive TcO.
锝-99(Tc)是一种长寿命放射性核素,对环境构成极大威胁,因此选择性地从水生系统中去除 Tc 一直是一个问题。氨甲基吡啶(AMP)配备吡啶和氨基,是 TcO 和其替代物 ReO 的有前途的受体,因此探索和理解与 n-AMP 结构中氨基甲基位置不同的 ReO 吸附的结构-性能关系很有意义。在这项工作中,合成了三种 n-AMP 功能化纤维素微球(n-AMPR,n=2,3,4),并用于 TcO/ReO 的摄取。研究并比较了氨基甲基位置对 n-AMPR 吸附 ReO 的影响。吸附动力学和吸附等温线表明,吸附速度和吸附容量的顺序为 3-AMPR>2-AMPR>4-AMPR。DFT 计算验证了 n-AMPR 对 ReO 的吸附归因于静电相互作用和氢键相互作用,n-AMPR 吸附能力的顺序是由于空间效应和氢键协同稳定了 n-AMPR-ReO 配合物。柱实验表明,3-AMPR 可从模拟地下水中选择性去除 ReO。更重要的是,Tc 柱实验表明,3-AMPR 对实际放射性 TcO 具有更好的去除能力。