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新型分级棒状 Mg-Al 双金属氧化物的合成及其增强废水中铀(VI)去除性能的研究。

Synthesis of Novel Hierarchical Rod-like Mg-Al bimetallic oxides for enhanced removal of uranium (VI) from wastewater.

机构信息

Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, 100 Daxue East Road, Nanning, 530004, PR China.

School of Nuclear Science and Technology, University of South China, 28 Changsheng West Road, Hengyang, 421001, PR China.

出版信息

Chemosphere. 2022 Dec;308(Pt 3):136546. doi: 10.1016/j.chemosphere.2022.136546. Epub 2022 Sep 21.

Abstract

As one of the most frequently used nuclides for nuclear fuel and toxic heavy metal in polluted solutions, the removal and recovery of U(VI) from wastewater is significant both for nuclear energy and human health. Herein, the novel hierarchical Mg-Al bimetallic oxides (Mg/Al-BOs) were successfully synthesized by a facile hydrothermal-lyophilization-calcination method for enhanced removal of uranium (U(VI)) from wastewater. The as-synthesized Mg/Al-BOs adsorbents were characterized by a variety of techniques including SEM-EDS, XRD, high temperature in-situ XRD, TG-DSC, N adsorption-desorption isotherm and XPS. Batch experiments including the effects of pH, hydration species, interfering ions on U(VI) removal, adsorption kinetics, isotherms and recyclability were systematically studied. Results showed that calcined Mg/Al-BO-24 inherited the hierarchical structure from its hydrotalcite-like precursor and grew the bimetallic oxides of AlO/MgO into a 3D rod-like and mesoporous network with the large BET surface area (472.4 m∙g-), which presented abundant binding sites on the surface and contributed to preventing the aggregation of AlO/MgO nanoparticles, allowing the fast uptake of U(VI) for equilibrium within 180 min and the significant increase of maximum adsorption capacity to 411.5 mg∙g-. The uptake kinetics and isotherms of U(VI) removal could be well represented by the pseudo-second-order and Langmuir models, respectively. Further, it was demonstrated that U(VI) removal by Mg/Al-BO-24 was less influenced by coexisting cations and the regeneration cycles, indicating the excellent selectivity and reusability for U(VI) by the as-prepared composites. Based on the XPS analysis results, the mechanisms for U(VI) sorption onto the Mg/Al-BO-24 were mainly ascribed to the synergistic surface complexation and electrostatic interaction. These results suggested that Mg/Al-BO-24 prepared by the method reported here was available for developing other multiple metal oxides and would be a promising material for the effective treatment of wastewater with U(VI)-contamination.

摘要

作为核燃料和污染溶液中有毒重金属的最常用核素之一,从废水中去除和回收 U(VI) 对于核能和人类健康都具有重要意义。在此,通过简便的水热-冻干-煅烧法成功合成了新型分层 Mg-Al 双金属氧化物 (Mg/Al-BO),用于增强废水中铀 (U(VI)) 的去除。所合成的 Mg/Al-BO 吸附剂通过 SEM-EDS、XRD、高温原位 XRD、TG-DSC、N 吸附-解吸等温线和 XPS 等多种技术进行了表征。系统研究了 pH、水合物种、共存离子对 U(VI)去除的影响、吸附动力学、等温线和可回收性等批量实验。结果表明,煅烧后的 Mg/Al-BO-24 继承了其类水滑石前体的分层结构,并将 AlO/MgO 双金属氧化物生长成 3D 棒状和中孔网络,具有较大的 BET 表面积 (472.4 m∙g-1),表面具有丰富的结合位点,有助于防止 AlO/MgO 纳米颗粒的聚集,使 U(VI)在 180 min 内达到平衡,最大吸附容量显著增加到 411.5 mg∙g-1。U(VI)去除的吸附动力学和等温线可以很好地用伪二阶和朗缪尔模型来表示。此外,还证明了 Mg/Al-BO-24 对共存阳离子和再生循环的 U(VI)去除影响较小,表明所制备的复合材料对 U(VI)具有优异的选择性和可重复使用性。基于 XPS 分析结果,U(VI)在 Mg/Al-BO-24 上的吸附机制主要归因于表面络合和静电相互作用的协同作用。这些结果表明,通过本文报道的方法制备的 Mg/Al-BO-24 可用于开发其他多种金属氧化物,并且将是处理 U(VI)污染废水的有前途的材料。

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