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功能化氨甲基吡啶异构体纤维素微球对 TcO/ReO 吸收的研究:结构-性能关系及其在不同水系统中的应用。

Aminomethylpyridine isomers functionalized cellulose microspheres for TcO/ReO uptake: Structure-properties relationship and their application in different aquatic systems.

机构信息

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.

出版信息

J Hazard Mater. 2022 Jul 5;433:128728. doi: 10.1016/j.jhazmat.2022.128728. Epub 2022 Mar 29.

DOI:10.1016/j.jhazmat.2022.128728
PMID:35364538
Abstract

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.

摘要

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。

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