正确的理由正确的答案? 基准测试协议和陷在一个Ru-metathesis的例子
Naziha Tarannam1, Nebal Alassad1, N Gabriel Lemcoff1,2
1Department of Chemistry, Ben-Gurion University of the Negev, Beer-Sheva 84105, Israel.
Journal of chemical theory and computation
|July 17, 2023
概括
为吉布斯能量选择计算方法需要仔细对所有组件进行基准测试,包括溶解和. 在有机金属化学中,准确地预测反应能量取决于计算和实验值的匹配.
科学领域:
- 计算化学计算化学
- 催化剂是一种催化剂.
- 物理化学 物理化学
背景情况:
- 准确的吉布斯能量估计对于理解和设计催化反应至关重要.
- 涉及鲁复合物的转化催化剂在有机合成中很重要.
- 计算化学的方法选择需要严格的验证.
研究的目的:
- 为吉布斯能量估计开发一个选择计算方法的协议.
- 对催化反应的实验数据进行计算方法的比较.
- 评估对有机金属复合物的各种计算方法的准确性.
主要方法:
- 分层的元基准分析分析结合了计算和实验数据.
- 气相能量计算使用DLPNO-CCSD(T) /CBS作为参考.
- 对和吉布斯能量的基准测试,包括溶解和效应.
- 评估不同的密度函数 (例如, ωB97XD,M06) 和溶解模型 (IEF-PCM,SMD).
主要成果:
- DLPNO-CCSD(T) /CBS是大型系统的可靠参考.
- ωB97XD 和 M06 函数证明了高精度.
- 溶解模型的选择取决于系统;IEF-PCM和SMD的性能各不相同.
- 低频振动对计算产生重大影响,需要调整切线参数.
- 溶解对于度至关重要,但对于度准确性不够.
结论:
- 对有机金属反应进行准确的吉布斯能量计算需要精确评估所有组件:电子能量,,和溶解.
- 一个全面的,分层的基准分析方法对于方法选择至关重要.
- 将计算的吉布斯能量项与基准实验和计算值相匹配,可以确保可靠的预测.
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