Fujian Key Laboratory of Pollution Control and Resource Reuse, School of Environmental and Resource Sciences, Fujian Normal University, Fuzhou 350117, Fujian, China.
Fujian Key Laboratory of Pollution Control and Resource Reuse, School of Environmental and Resource Sciences, Fujian Normal University, Fuzhou 350117, Fujian, China.
J Hazard Mater. 2024 Dec 5;480:136320. doi: 10.1016/j.jhazmat.2024.136320. Epub 2024 Oct 26.
Iron nanoparticles synthesized using Euphorbia cochinchinensis leaf extracts (Ec-FeNPs) showed high selectivity for rare earth elements (REEs) recovery from mining wastewater. REEs recovery efficiencies were > 90 %, with distribution coefficients ranging from 2483.9 to 37500 mL/g, which were consistently much higher than non-REEs (15.0 - 234.8 mL/g). Moreover, even after 5 consecutive reuse cycles, Ec-FeNPs effectively adsorbed > 60 % of REEs. Application of advanced characterization techniques found that the high selectivity of Ec-FeNPs for REEs was mainly due to the biomolecules present in the Ec extract. During the synthesis of FeNPs, these biomolecules are modified on the surface of Ec-FeNPs, giving Ec-FeNPs an enhanced ability to separate REEs from non-REEs. The biomolecule capping layer, which is modified on the surface of Ec-FeNPs, constitutes a primary source of high selectivity. LC-MS identified amino acids, carbohydrates, and organic acids as the major biomolecule categories in the capping layer. Density functional theory (DFT) confirmed that the biomolecule capping layer of Ec-FeNPs had the strongest interaction with REEs; an association confirmed by Spearman's correlation analysis. The adsorption mechanism of REEs by Ec-FeNPs mainly involved a combination of ion exchange, electrostatic adsorption, and surface complexation. Overall, the novel findings reported here provide new perspectives for the design of absorbents with highly selective recovery of REEs from mining wastewater.
使用大戟叶提取物合成的铁纳米粒子(Ec-FeNPs)对从矿山废水中回收稀土元素(REEs)具有很高的选择性。REEs 的回收效率>90%,分配系数范围为 2483.9 至 37500 mL/g,明显高于非 REEs(15.0-234.8 mL/g)。此外,即使经过 5 次连续重复使用循环,Ec-FeNPs 仍能有效地吸附>60%的 REEs。先进的表征技术应用发现,Ec-FeNPs 对 REEs 的高选择性主要归因于 Ec 提取物中存在的生物分子。在 FeNPs 的合成过程中,这些生物分子会被修饰在 Ec-FeNPs 的表面,使 Ec-FeNPs 具有从非 REEs 中分离 REEs 的增强能力。修饰在 Ec-FeNPs 表面的生物分子覆盖层是高选择性的主要来源。LC-MS 鉴定出氨基酸、碳水化合物和有机酸是覆盖层中主要的生物分子类别。密度泛函理论(DFT)证实,Ec-FeNPs 的生物分子覆盖层与 REEs 具有最强的相互作用;Spearman 相关性分析证实了这种关联。Ec-FeNPs 吸附 REEs 的机制主要涉及离子交换、静电吸附和表面络合的结合。总的来说,这里报道的新发现为设计从矿山废水中高度选择性回收 REEs 的吸附剂提供了新的视角。