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层状双氢氧化物插层二乙烯三胺五乙酸对 Mn(II)的高效吸附及机理研究。

Efficient adsorption of Mn(II) by layered double hydroxides intercalated with diethylenetriaminepentaacetic acid and the mechanistic study.

机构信息

School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.

School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China; Key Laboratory of Water and Wastewater Treatment (HUST), MOHURD, Wuhan 430074, China.

出版信息

J Environ Sci (China). 2019 Nov;85:56-65. doi: 10.1016/j.jes.2019.04.011. Epub 2019 Apr 25.

DOI:10.1016/j.jes.2019.04.011
PMID:31471031
Abstract

In this study, greatly enhanced Mn(II) adsorption was achieved by as-synthesized diethylenetriaminepentaacetate acid intercalated Mg/Al layered double hydroxides (LDHs-DTPA). The adsorption capacity of LDHs-DTPA was 83.5 mg/g, which is much higher than that of LDHs-EDTA (44.4 mg/g), LDHs-Oxalate (21.6 mg/g) and LDHs (28.8 mg/g). The adsorption data of aqueous Mn(II) using LDHs-DTPA could be well described by the pseudo-second order kinetics and Langmuir isotherm model. Thermodynamics study results also showed that the adsorption process of Mn(II) by LDHs-DTPA was exothermic as indicated by the negative ΔH value. Furthermore, based on the structural, morphological and thermostable features, as well as FT-IR and XPS characterizations of LDHs-DTPA and the pristine LDHs, the adsorption mechanism of Mn(II) was proposed. The carboxyl groups of DTPA were proposed to be the main binding sites for Mn(II), and the hydroxyl groups of LDHs also played a minor role in the adsorption process. Among the three common regeneration reagents, 0.1 mol/L NaCO was the best for reusing LDHs-DTPA in Mn(II) adsorption. Besides, the Mn(II) adsorption performance could be hindered in the presence of typical inorganic ions, especially cations. Further specific modifications of LDHs-DTPA are suggested to get more selective adsorption of Mn(II) in practical applications.

摘要

在这项研究中,通过合成的二乙三胺五乙酸酸插层镁/铝层状双氢氧化物(LDHs-DTPA)实现了 Mn(II) 的吸附性能的显著提高。LDHs-DTPA 的吸附容量为 83.5 mg/g,远高于 LDHs-EDTA(44.4 mg/g)、LDHs-草酸盐(21.6 mg/g)和 LDHs(28.8 mg/g)。LDHs-DTPA 对水溶液中 Mn(II) 的吸附数据可以很好地用伪二级动力学和 Langmuir 等温线模型来描述。热力学研究结果还表明,Mn(II)通过 LDHs-DTPA 的吸附过程是放热的,这表明ΔH 值为负。此外,基于 LDHs-DTPA 和原始 LDHs 的结构、形态和热稳定性特征,以及 FT-IR 和 XPS 表征,提出了 Mn(II)的吸附机理。提出 DTPA 的羧基是与 Mn(II)结合的主要位点,而 LDHs 的羟基在吸附过程中也起次要作用。在三种常见的再生试剂中,0.1 mol/L 的 NaCO 是再利用 LDHs-DTPA 吸附 Mn(II)的最佳试剂。此外,Mn(II)的吸附性能可能会受到典型无机离子的阻碍,尤其是阳离子。建议对 LDHs-DTPA 进行进一步的特定修饰,以在实际应用中获得对 Mn(II)的更选择性吸附。

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