用密度泛函活性理论和Hammett常数预测单双取代苯酚的酸性(英文)

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用从头算和密度泛函理论准确预测分子的酸碱性仍然是一个悬而未决的理论和计算难题.近年来运用密度泛函活性理论(DFRT)发展的分子静电势和价自然原子轨道等概念为该问题的解决提供了一个简单而有效的途径.最近我们还提出用Hammett常数预测分子酸碱性,并发现对苯甲酸衍生物其预测精度与DFRT方法一致.本文将这两个新方法运用于苯酚衍生物体系以验证其普适性,一共计算了83个体系.发现二者均可以得到较好的预测精度,且DFRT方法比Hammett常数结果稍好.对进一步从局部和整体角度理解分子性质的起源以及这些性质的决定因素提供了有益启示.该文同时还验证了Hammett常数求和规则的普适性. It is still a pending theoretical and computational challenge to predict the acidity and alkalinity of a molecule accurately using ab initio and density functional theory.In recent years the concepts of molecular electrostatic potential and valence atomic orbitals developed by using density functional theory (DFRT) The solution of the problem provides a simple and effective way.We have also recently proposed using the Hammett constant to predict the molecular acidity and alkalinity, and found that the prediction accuracy of benzoic acid derivatives is consistent with the DFRT method.In this paper, these two new methods were applied to phenol Derivative system to verify its universality, a total of 83 systems were calculated .It was found that both can get better prediction accuracy, and the DFRT method slightly better than the Hammett constant results.For further from the partial and overall understanding of the molecular nature The origin and the determinants of these properties.It also verifies the universality of Hammett’s constant summation rules.
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