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Application of hybrid MOF composite in extraction of f-block elements: Experimental and computational investigation
Chemosphere ( IF 8.1 ) Pub Date : 2021-09-09 , DOI: 10.1016/j.chemosphere.2021.132232
Gauri Salunkhe 1 , Arijit Sengupta 2 , Anil Boda 3 , Roxana Paz 4 , Nishesh Kumar Gupta 5 , Carolina Leyva 4 , Rohit Singh Chauhan 3 , Sk Musharaf Ali 6
Affiliation  

An attempt was made to understand the sorption behaviour of UO22+, Th4+ and Eu3+ on novel hybrid metal-organic framework composites, FeBDC@CoBDC. The XRD pattern revealed the composite nature of the hybrid MOF materials, while FTIR and Raman spectroscopic analyses evidenced the presence of different functional moieties. The thermal stability of the hybrid MOF composites was investigated through thermogravimetric analysis. The sorption predominantly followed Langmuir isotherm with sorption capacity of 189 mg g−1, 224 mg g−1 and 205 mg g−1 for UO22+, Th4+ and Eu3+ respectively. The sorption proceeded through chemisorption following pseudo 2nd order rate kinetics. The processes were found to be thermodynamically favourable and endothermic in nature. However, they were entropically driven. Multiple contacts of complexing agents were necessary for quantitative elution of f-elements from loaded MOF. The MOF showed moderate stability towards radiation exposure. DFT calculation was used for the optimization of structures, estimation of bond length and estimation of binding energy. In hybrid MOF composites, the Fe atom was having six coordination with 4 O atoms of BDC moieties and 2 O atoms of –OH groups. The O atoms of BDC and –OH groups were coordinated to Eu, Th and U atoms during their sorption.



中文翻译:

混合 MOF 复合材料在 f 块元素提取中的应用:实验和计算研究

试图了解 UO 2 2+、Th 4+和 Eu 3+在新型混合金属有机骨架复合材料 FeBDC@CoBDC 上的吸附行为。XRD 图揭示了混合 MOF 材料的复合性质,而 FTIR 和拉曼光谱分析证明存在不同的功能部分。通过热重分析研究了混合 MOF 复合材料的热稳定性。吸附主要遵循朗缪尔等温线,对 UO 2 2+、Th 4+和 Eu 3+ 的吸附容量分别为 189 mg g -1、224 mg g -1和 205 mg g -1分别。吸附通过化学下面的伪2进行第二阶速率动力学。发现这些过程在热力学上是有利的并且本质上是吸热的。然而,它们是熵驱动的。从负载的 MOF 中定量洗脱 f 元素需要络合剂的多次接触。MOF 对辐射暴露表现出中等稳定性。DFT 计算用于优化结构、估计键长和估计结合能。在混合 MOF 复合材料中,Fe 原子与 BDC 部分的 4 个 O 原子和 -OH 基团的 2 个 O 原子具有六个配位。BDC 和 -OH 基团的 O 原子在吸附过程中与 Eu、Th 和 U 原子配位。

更新日期:2021-09-23
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