用电子结构方法预测晚期乙化物Cm到Lr的还氧化潜力
Felipe R Dutra1,2, David A Dixon2
1Instituto de Química, Universidade Estadual de Campinas, Barão Geraldo, 13083-970 Campinas, São Paulo, Brazil, P.O. Box 6154.
The journal of physical chemistry. A
|November 11, 2025
概括
这项研究扩展了计算方法,以预测后来的活性化物的水性氧化还原潜力,在使用密度函数理论和溶解模型的许多氧化还原配对中达到±0.2V的精度.
科学领域:
- 计算化学是一种计算化学.
- 动氨基酸的化学成分
- 物理化学 物理化学
背景情况:
- 之前为早期的动因化物开发了先前的计算方法.
- 延伸到后来的动因化物:Cm,Bk,Cf,Es,Fm,Md,No,Lr.
- 准确的氧化还原电位计算对于理解活性化物行为的重要性.
研究的目的:
- 为了将水性氧化还原潜力的计算方法扩展到以后的活性化物.
- 用不同的溶解模型评估密度函数理论 (DFT) 的准确性.
- 在实验数据稀缺的情况下,提供可靠的氧化还原潜力预测.
主要方法:
- 密度函数理论 (DFT) 具有小核心伪潜力.
- 使用30个水分子进行溶解的超分子连续体方法.
- 在COSMO和SMD隐式解决模型中.
- 包括旋转轨道校正以提高准确度.
主要成果:
- 计算和实验结构参数以及Cm{\displaystyle Cm} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Cf{\displaystyle Cf} 的水合数与Cm{\displaystyle Cm} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} ,Bk{\displaystyle Bk} 和Cf{\displaystyle Cf{\displaystyle Cf} .
- B3LYP/COSMO方法预测大多数氧化对的氧化还原电位在±0.2V以内.
- 旋转轨道校正改善了在高氧化状态下较晚的活性化物的结果.
- 计算的An(III/0) 潜力与使用COSMO和NIST电离能量的实验数据最一致.
结论:
- 扩展的计算方法准确地预测了后来的活性化物的水性氧化还原潜力.
- 具有适当的溶解模型 (COSMO,SMD) 和旋转轨道校正的DFT是预测动因子氧化还原潜力的可靠工具.
- 这项研究为了解这些具有挑战性的元素的化学成分提供了宝贵的数据.
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