Theoretical Exploration of the Synergistic Effect of Phosphate and Amidoxime for Uranium Recovery from Seawater

化学 海水 磷酸盐 环境化学 核化学 无机化学 有机化学 冶金 海洋学 地质学 材料科学
作者
Yichen Huang,Cong-Zhi Wang,Qun‐Yan Wu,Jian‐Hui Lan,Changming Nie,Shusen Chen,Yan Song,Hao Li,Wei‐Qun Shi
出处
期刊:Inorganic Chemistry [American Chemical Society]
卷期号:63 (52): 24685-24696
标识
DOI:10.1021/acs.inorgchem.4c03912
摘要

Highly selective extraction of uranium from seawater is currently extremely challenging. Although the amidoxime group (HAO) is the commonly used ligand in seawater uranium extraction, it also has strong binding capacity for vanadium ion. It has been shown that the introduction of phosphate groups into amidoxime-based adsorbents can improve the adsorption performance of materials through a synergistic effect between functional groups. In this work, we have systematically investigated the selective extraction behavior of the phosphate ligand (methylphosphonic acid, HL1) for uranyl cation and the synergistic effect with amidoxime using density functional theory (DFT). The electron-donor-substituted derivatives of HL1 (aminomethylphosphonic acid (HL2) and methyl phosphate (HL3)) were also considered. Not unexpectedly, the results show that introduction of HL1 into the amidoxime-based adsorbents improves the extraction and selectivity for uranyl cations. This is mainly due to the fact that HL1 is more likely to deprotonate, which promotes the dissociation of [UO2(CO3)3]4–, and the presence of the phosphate groups in the synergistic complexes alters the optimal coordination mode of VO2+. In addition, the HL2 and HL3 ligands further improve the uranium extraction performance, especially for HL3. This work provides guidelines for the rational design of sequestering ligands for uranium extraction from seawater.
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