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理性设计的二齿酸根功能化二氧化硅用于从电子废物中高效回收稀土元素。

Rationally designed dipicolinate-functionalized silica for highly efficient recovery of rare-earth elements from e-waste.

机构信息

Pontifical Catholic University of Rio de Janeiro, Marquês de São Vicente St. 225, Rio de Janeiro 22451-900, Brazil.

Pontifical Catholic University of Rio de Janeiro, Marquês de São Vicente St. 225, Rio de Janeiro 22451-900, Brazil; National University of Kyiv-Mohyla Academy, 2 Skovorody vul., Kyiv 04070, Ukraine.

出版信息

J Hazard Mater. 2021 Apr 15;408:124976. doi: 10.1016/j.jhazmat.2020.124976. Epub 2020 Dec 28.

Abstract

Composition of the immobilized layer plays a crucial role in metal adsorption properties of complexing organo-mineral materials. Ignoring the specific features of chemical reactions on solid surface can lead to a significant deterioration in the target properties of the resulted materials. In this research we demonstrated that rationally designed surface-assembling synthesis of organo-silica with covalently immobilized fragments of dipicolinic acid (DPA) resulted in the adsorbent that is capable quantitively recover almost all Rare Earth elements (REEs) from multielement solution with pH > 1.7. In ten consecutive adsorption/desorption cycles no noticeable loss of its efficiency was found, with a mean value of REEs recovery larger than 97%. The adsorbent has been used to recover REEs from model solutions (22 metal ions in 0.5 mol L NaCl) and real leaching solution of waste of fluorescent lamps. It was demonstrated that even 3200-fold excess of Fe and Cu ions only slightly reduces REEs recovery. The adsorbent is capable to recover above 80% of all (except La) REEs from acidic leaching solution from fluorescent lamps with enrichment factors above 600. After adsorption of Eu and Tb, the resulting materials exhibited strong red and green luminescence, respectively, indicating chelating mechanism of REEs adsorption on SiO-DPA.

摘要

固定化层的组成在配位有机-矿物材料的金属吸附性能中起着至关重要的作用。如果忽略固体表面化学反应的具体特点,可能会导致所得材料的目标性能显著恶化。在这项研究中,我们证明了通过合理设计的表面组装合成方法,将共价固定化的二吡啶酸(DPA)片段接枝到有机硅上,得到了一种吸附剂,它能够在 pH>1.7 的多元素溶液中定量回收几乎所有的稀土元素(REEs)。在十个连续的吸附/解吸循环中,没有发现其效率有明显损失,REEs 的平均回收率大于 97%。该吸附剂已用于从模型溶液(0.5 mol L NaCl 中 22 种金属离子)和荧光灯废物的实际浸出溶液中回收 REEs。结果表明,即使有 3200 倍过量的 Fe 和 Cu 离子,也只会轻微降低 REEs 的回收率。该吸附剂能够从荧光灯的酸性浸出溶液中回收超过 80%的除 La 以外的所有 REEs,富集因子超过 600。Eu 和 Tb 吸附后,所得材料分别表现出强的红色和绿色发光,表明 REEs 在 SiO-DPA 上的吸附是螯合机理。

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