Deuterated Malonamide Synthesis for Fundamental Research on Solvent Extraction Systems
Deuterated Malonamide Synthesis for Fundamental Research on Solvent Extraction Systems
复制标题
用于溶剂萃取系统基础研究的氘代丙二酰胺合成
DOI：
10.1080/07366299.2023.2166351
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发表时间：
2023
影响因子：
2
通讯作者：
Motokawa Ryuhei
中科院分区：
文献类型：
--
作者：
Micheau Cyril;Ueda Yuki;Akutsu-Suyama Kazuhiro;Bourgeois Damien;Motokawa Ryuhei
丙二酰胺衍生物，这是最广泛的研究萃取剂的溶剂萃取镧系元素，锕系元素，和铂族金属离子，氘代通过使用Pd/C和Rh/C催化剂中的D2 O/2-丙醇混合物。该方法以可控的氘代速率将丙二酰胺中的1H原子与2 H原子进行氘代反应。通过核磁共振和电喷雾电离质谱测定，最大转化率达到75%左右.丙二酰胺对金属离子的萃取行为不受氘代的影响。氘代丙二酰胺是溶剂萃取体系基础研究和有机相结构分析的有力工具。1H和2 H的中子相干散射截面的巨大差异导致了丙二酰胺衍生物氘代前后中子散射长度密度的巨大差异。因此，在小角中子散射和中子反射率研究中使用氘代丙二酰胺可能有助于分别揭示本体有机相中和液-液界面处的特定溶质物种的微观结构。本文报道了氘代丙二酰胺作为对比度匹配方法在SANS实验中的优势。这种氘代方法可以推广和扩展到各种各样的萃取剂分子。
Malonamide derivatives, which are the most extensively investigated extractants for solvent extraction of lanthanides, actinides, and platinum group metal ions, were deuterated by using Pd/C and Rh/C catalysts in a D2O/2-propanol mixture. This method replaces1H atoms in the malonamides with2H atoms at a controllable deuteration rate. The maximum rate reached about 75%, determined by nuclear magnetic resonance and electrospray ionization – mass spectrometry. The extraction behavior of metal ions by the malonamides was unchanged by the deuteration. Deuterated malonamides are a powerful tool for fundamental research on solvent extraction systems and for structural analysis of organic phases. The large difference in the cross section of coherent neutron scattering between1H and2H leads to a large difference in neutron scattering length density of malonamide derivatives before and after the deuteration. Therefore, using deuterated malonamides in small-angle neutron scattering and neutron reflectivity studies may help to reveal the microscopic structure of the specific solute species in the bulk organic phase and at the liquid–liquid interface, respectively. In this paper, we report the advantage of the deuterated malonamides for a contrast-matching method in the SANS experiment. This deuteration method could be generalized and extended to a wide variety of extractant molecules.