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二乙烯三胺功能化亚马逊高岭土对 U(VI)的去除:阳离子-碱性相互作用的热力学。

Amazon kaolinite functionalized with diethylenetriamine moieties for U(VI) removal: thermodynamic of cation-basic interactions.

机构信息

Universidade Federal de Mato Grosso, UFMT, Centro de Recursos Minerais, Cuiabá, Mato Grosso, Brazil.

出版信息

J Hazard Mater. 2010 Aug 15;180(1-3):683-92. doi: 10.1016/j.jhazmat.2010.04.092. Epub 2010 Apr 29.

Abstract

The compound N-[3-(trimethoxysilyl)propyl]diethylenetriamine (MPDET) was anchored onto Amazon kaolinite surface (KLT) by heterogeneous route. The modified and natural kaolinite clay samples were characterized by transmission electron microscopy (TEM), scanning electron microscopic (SEM), N(2) adsorption, powder X-ray diffraction, thermal analysis, ion exchange capacities, and nuclear magnetic nuclei of (29)Si and (13)C. The well-defined peaks obtained in the (13)C NMR spectrum in the 5.0-62.1 ppm region confirmed the attachment of organic functional groups as pendant chains bonded into the porous clay. The adsorption of uranyl on natural (KLT) and modified (KLT(MPDET)) kaolinite clays was investigated as a function of the solution pH, metal concentration, temperature, and ionic strength. The ability of these materials to remove U(VI) from aqueous solution was followed by a series of adsorption isotherms adjusted to a Sips equation at room temperature and pH 4.0. The maximum number of moles adsorbed was determined to be 8.37 x 10(-3) and 13.87 x 10(-3) mmol g(-1) for KLT and KLT(MPDET) at 298 K, respectively. The energetic effects (Delta(int)H, Delta(int)G, and Delta(int)S) caused by metal cations adsorption were determined through calorimetric titrations.

摘要

化合物 N-[3-(三甲氧基硅基)丙基]二亚乙基三胺 (MPDET) 通过非均相途径锚定到亚马逊高岭石表面 (KLT) 上。改性和天然高岭石粘土样品通过透射电子显微镜 (TEM)、扫描电子显微镜 (SEM)、N(2)吸附、粉末 X 射线衍射、热分析、离子交换容量和 (29)Si 和 (13)C 的核磁共振核进行了表征。在 5.0-62.1 ppm 区域获得的 (13)C NMR 谱中的明确峰证实了有机官能团的附着,作为支链键合到多孔粘土中。研究了天然 (KLT) 和改性 (KLT(MPDET)) 高岭石粘土对铀酰的吸附作为溶液 pH、金属浓度、温度和离子强度的函数。通过一系列吸附等温线来跟踪这些材料从水溶液中去除 U(VI)的能力,这些等温线在室温下和 pH 4.0 下调整到 Sips 方程。在 298 K 下,KLT 和 KLT(MPDET) 的最大吸附摩尔数分别为 8.37 x 10(-3) 和 13.87 x 10(-3) mmol g(-1)。通过量热滴定确定了金属阳离子吸附引起的能量效应 (Delta(int)H、Delta(int)G 和 Delta(int)S)。

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