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Toward Molecular Recognition of REEs: Comparative Analysis of Hybrid Nanoadsorbents with the Different Complexonate Ligands EDTA, DTPA, and TTHA
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1021/acs.inorgchem.7b02056
Elizabeth Polido Legaria 1 , Michail Samouhos 1 , Vadim G. Kessler 1 , Gulaim A. Seisenbaeva 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1021/acs.inorgchem.7b02056
Elizabeth Polido Legaria 1 , Michail Samouhos 1 , Vadim G. Kessler 1 , Gulaim A. Seisenbaeva 1
Affiliation
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Highly efficient tailored SiO2-based nanoadsorbents were synthesized for the selective extraction of rare-earth elements (REEs). Three different complexonates (EDTA, DTPA, and TTHA) were investigated in terms of uptake capacity and selectivity, showing capacities of up to 300 mg of RE3+/g and distinct preferential trends depending on the complexonate. EDTA-functionalized nanoadsorbents showed higher uptake for Dy3+, DTPA-functionalized ones for Nd3+, and TTHA-functionalized ones for La3+. The selectivity was even more pronounced in desorption at pH 3, with separation factors of up to 76 in ternary mixtures. A broad comparative study of single-crystal structures of the complexes between REE and the nongrafted complexonates at different pHs led to a molecular understanding of their individual modes of action. EDTA-derived nanoadsorbents combine concerted action and chelation, whereas the latter is the preferential coordination mechanism for DTPA- and TTHA-derived nanoadsorbents. These different mechanisms result in quite specific REE affinities, which opens great possibilities toward molecular recognition of REEs and for tailoring nanoadsorbents for a particular REE or group of REEs in their production from minerals and in recycling. It also brings new insights into how REEs are adsorbed on nanomaterials applied in a broad variety of fields, including bioimaging and MRI.
中文翻译：
稀土元素的分子识别：混合纳米吸附剂与不同络合物配体EDTA，DTPA和TTHA的比较分析
合成了高效定制的SiO 2基纳米吸附剂，用于选择性萃取稀土元素（REEs）。研究了三种不同的络合物（EDTA，DTPA和TTHA）的吸收能力和选择性，显示出高达300 mg RE 3+ / g的容量，并且取决于络合物具有明显的优先趋势。EDTA功能化的纳米吸附剂对Dy 3+的吸收更高，DTPA功能化的对Nd 3+的吸收，而TTHA功能化的对La 3+的吸收。。在pH为3的解吸中，选择性更为显着，三元混合物中的分离系数高达76。REE和非接枝的络合物在不同pH下对络合物的单晶结构进行了广泛的比较研究，从而使人们对它们各自的作用方式有了分子的了解。EDTA衍生的纳米吸附剂将协同作用和螯合结合在一起，而后者是DTPA和TTHA衍生的纳米吸附剂的优先配位机制。这些不同的机制导致非常特定的REE亲和力，这为REE的分子识别和为从矿物生产和循环利用中的特定REE或一组REE定制纳米吸附剂提供了极大的可能性。
更新日期：2017-10-30
中文翻译：
稀土元素的分子识别：混合纳米吸附剂与不同络合物配体EDTA，DTPA和TTHA的比较分析
合成了高效定制的SiO 2基纳米吸附剂，用于选择性萃取稀土元素（REEs）。研究了三种不同的络合物（EDTA，DTPA和TTHA）的吸收能力和选择性，显示出高达300 mg RE 3+ / g的容量，并且取决于络合物具有明显的优先趋势。EDTA功能化的纳米吸附剂对Dy 3+的吸收更高，DTPA功能化的对Nd 3+的吸收，而TTHA功能化的对La 3+的吸收。。在pH为3的解吸中，选择性更为显着，三元混合物中的分离系数高达76。REE和非接枝的络合物在不同pH下对络合物的单晶结构进行了广泛的比较研究，从而使人们对它们各自的作用方式有了分子的了解。EDTA衍生的纳米吸附剂将协同作用和螯合结合在一起，而后者是DTPA和TTHA衍生的纳米吸附剂的优先配位机制。这些不同的机制导致非常特定的REE亲和力，这为REE的分子识别和为从矿物生产和循环利用中的特定REE或一组REE定制纳米吸附剂提供了极大的可能性。
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