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首页> 外文期刊>The Journal of Supercritical Fluids >Extraction of metal ions with non-fluorous bipyridine derivatives as chelating ligands in supercritical carbon dioxide
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Extraction of metal ions with non-fluorous bipyridine derivatives as chelating ligands in supercritical carbon dioxide

机译：以非氟联吡啶衍生物为螯合配体在超临界二氧化碳中萃取金属离子

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摘要

Three new non-fluorous bipyridine derivatives, bis(2-(2-butoxyethoxy)ethyl)-2,2'-bipyridine-4,4'-dicarboxylate (ligand 1), bis(2-(2-ethoxyethoxy)ethyl)-2,2'-bipyridine-4,4'-dicarboxylate (ligand 2), and bis(2-butoxyethyl)-2,2'-bipyridine-4,4'-dicarboxylate (ligand 3), were synthesized as chelating ligands to remove metal ions from solid matrix into supercritical CO_2 (scCO_2). These produced compounds 1-3 showed considerable solubilities in scCO_2 (8.0 g/l, 4.8 g/l, 7.8 g/l for ligands 1-3 at 313 K, respectively) and the tested solubility data were then calculated and correlated with semiempirical model at different pressures and temperatures, which showed satisfactory agreement with each other and the average absolute relative deviation were in the range of 0.1-28.3%. The effects of pressure, temperature, time, and ligand to metal ratio (5:1 to 75:1) on the extraction efficiency of metal ions were also systematically investigated. The extraction efficiency was 100% for Ni~(2+) and 95.9% for Cu~(2+) in scCO_2 with the system of ligand 1, ultra-pure water, and perfluoro-1-octanesulfonic acid tetraethylammonium salt (PFOAT) under the optimized conditions (25 MPa, 313 K, 90 min, and ligand to metal ratio of 10). Although all ligands exhibited good efficiency for Ni~(2+) ( > 85%) and Cu~(2+) ( > 70%) extraction, the extraction of mixed metal ions indicated that the bipyridine derivatives had low selectivity. Finally, the detailed calculation results exhibited that the extraction constants (K_(ex)) of the metal ions increased with the increase of the extraction efficiency in the same extraction system for each same metal ion.
机译：三种新的非氟联吡啶衍生物，双（2-（2-丁氧基乙氧基）乙基）-2,2'-联吡啶-4,4'-二羧酸酯（配体1），双（2-（2-乙氧基乙氧基）乙基）-合成了2,2'-联吡啶-4,4'-二羧酸盐（配体2）和双（2-丁氧基乙基）-2,2'-联吡啶-4,4'-二羧酸盐（配体3）作为螯合配体从固体基质中去除金属离子成超临界CO_2（scCO_2）。这些生成的化合物1-3在scCO_2中显示出可观的溶解度（配体1-3在313 K下分别为8.0 g / l，4.8 g / l，7.8 g / l），然后计算测试的溶解度数据并将其与半经验模型相关在不同的压力和温度下，彼此显示出令人满意的一致性，并且平均绝对相对偏差在0.1-28.3％的范围内。还系统地研究了压力，温度，时间以及配体与金属的比例（5：1至75：1）对金属离子萃取效率的影响。在配体1，超纯水和全氟-1-辛磺酸四乙铵盐（PFOAT）的体系下，scCO_2中Ni〜（2+）的萃取效率为100％，Cu〜（2+）的萃取率为95.9％。优化的条件（25 MPa，313 K，90分钟，配体与金属的比例为10）。尽管所有配体对Ni〜（2+）（> 85％）和Cu〜（2+）（> 70％）的萃取均表现出良好的效率，但混合金属离子的萃取表明联吡啶衍生物的选择性较低。最后，详细的计算结果表明，对于相同的金属离子，在相同的萃取系统中，金属离子的萃取常数（K_（ex））随着萃取效率的提高而增加。

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