论文部分内容阅读
钚是最重要的放射性核素之一,Pu(IV)与有机还原的的氧化还原反应一直是核燃料后处理研究的重点之一。通过肼衍生物结构与Pu(IV)还原速率之间构效关系的研究,获得其关键影响因素,为镎钚分离提供关键数据及研究方向指引。采用密度泛函B3LYP方法和6-311+(3d,3p)基组对11种肼衍生物进行了几何优化和能量计算,获得了其最稳定构型。并利用Hyper Chem软件包计算优化后的分子的疏水性参数等结构描述符。运用数学统计软件SPSS对相应的物理化学参数进行相关性分析及逐步回归分析,最终得到具有良好相关性的构效关系(Quantitative structure-activity relationships,QSAR)方程。方程表明,疏水性参数是影响肼衍生物对Pu(IV)还原速率的主要因素,且与Pu(IV)还原速率呈负相关。
Plutonium is one of the most important radionuclides. Pu (IV) and organic reduction redox reactions have been one of the focuses of nuclear fuel reprocessing. Through the study of the structure-activity relationship between the structure of the hydrazine derivative and the reduction rate of Pu (IV), the key influencing factors were obtained, which provided the key data and guidelines for the separation of plutonium from plutonium. The 11 kinds of hydrazine derivatives were geometrically optimized and energetically calculated using the density functional B3LYP method and the 6-311 + (3d, 3p) basis set. The most stable configuration was obtained. And use the Hyper Chem software package to calculate structural descriptors such as the optimized hydrophobic parameter of the molecule. The correlation analysis and stepwise regression analysis of corresponding physicochemical parameters were carried out by using the mathematical statistical software SPSS to finally obtain the QSAR equation with good correlation. The equation shows that the hydrophobic parameter is the main factor affecting the reduction rate of Pu (IV) by hydrazine derivatives, and is negatively correlated with the reduction rate of Pu (IV).