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化学固载和物理吸附的 PAN/乙酰丙酮修饰介孔硅用于从废水中回收稀土元素的比较和优化研究。

Chemically immobilized and physically adsorbed PAN/acetylacetone modified mesoporous silica for the recovery of rare earth elements from the waste water-comparative and optimization study.

机构信息

Laboratory of Green Chemistry, Lappeenranta University of Technology, Mikkeli FI-50130, Finland.

Laboratory of Green Chemistry, Lappeenranta University of Technology, Mikkeli FI-50130, Finland.

出版信息

Water Res. 2017 May 1;114:264-276. doi: 10.1016/j.watres.2017.02.045. Epub 2017 Feb 20.

DOI:10.1016/j.watres.2017.02.045
PMID:28254644
Abstract

This study was aimed at the investigation of Rare Earth Element (REE) recovery from aqueous solution by silica gels with 1-(2-Pyridylazo) 2-naphthol (PAN) and acetyl acetone (Acac) modifications. The two different methods of silica gel chelation, such as chemical immobilization with the help of silane coupling agents (3-aminopropyl triethoxysilane (APTES) and 3-aminopropyl trimethoxysilane (APTMS) in this study) and direct physical adsorption onto the silica surface, is compared in terms of their REE removal efficiency. A comparative analysis between adsorption of different REEs for different silica gels is performed and the influence of parameters such as pH, contact time, temperature and initial concentration has been reported. The effect of calcined adsorbents on the adsorption process is also investigated. Characterization studies on silica gels by Fourier transform infrared spectroscopy (FTIR), Scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD) and zeta potential analysis are performed to better understand the relation between physical/chemical attributes of the adsorbents and their impact on the adsorption process. The experimental results are evaluated and optimal conditions for REE adsorption are identified. Chemically immobilized gels demonstrated immense potential for all the REE under study except Sc, for which, physically loaded gels seemed to be more efficient. The removal of REEs could be achieved at lower pHs by chemically immobilized PAN/Acac gels, making it suitable for many practical applications. The amine functionalized gels before chemical immobilization step were compared with PAN/Acac chemically immobilized gels in single as well as multi element system and the significance of chemical immobilization after amine functionalization is also stated.

摘要

本研究旨在研究硅胶通过 1-(2-吡啶偶氮)-2-萘酚(PAN)和乙酰丙酮(Acac)修饰从水溶液中回收稀土元素(REE)。本研究比较了两种不同的硅胶螯合方法,即化学固定化(使用硅烷偶联剂 3-氨丙基三乙氧基硅烷(APTES)和 3-氨丙基三甲氧基硅烷(APTMS))和直接物理吸附到硅胶表面,比较了它们的 REE 去除效率。对不同硅胶对不同 REE 的吸附进行了比较分析,并报告了 pH、接触时间、温度和初始浓度等参数的影响。还研究了煅烧吸附剂对吸附过程的影响。通过傅里叶变换红外光谱(FTIR)、扫描电子显微镜(SEM)、BET、X 射线衍射(XRD)和zeta 电位分析对硅胶进行了表征研究,以更好地理解吸附剂的物理/化学性质与其对吸附过程的影响之间的关系。对实验结果进行了评估,并确定了 REE 吸附的最佳条件。除 Sc 外,化学固定化凝胶对所有研究的 REE 都表现出巨大的潜力,而对于 Sc,物理负载凝胶似乎更有效。通过化学固定化的 PAN/Acac 凝胶,可以在较低的 pH 值下实现 REE 的去除,使其适用于许多实际应用。在单元素和多元素体系中,比较了胺功能化凝胶在化学固定化前与 PAN/Acac 化学固定化凝胶的性能,阐明了胺功能化后化学固定化的意义。

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