电子结构理论方法、热力学和隐式溶解修正对有机碳酸盐构象和结合能的影响

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Alexander S. Ryzhako, Anna A. Tuma, Arseniy A. Otlyotov, Yury Minenkov
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引用次数: 0

摘要

本研究探讨了电子结构或力场方法、气相热力学校正以及连续介质溶解模型对有机碳酸盐团簇 (S)n 构象和结合能的影响。测试的力场方法(GFN-FF、GAFF、MMFF94)和标准半经验方法(PM3、AM1、RM1、PM6、PM6-D3、PM6-D3H4、PM7)都不能再现参考的 RI-SCS-MP2 构象能。紧密结合 GFNn-xTB 方法提供了更真实的构象能,其精确度足以舍弃最不稳定的构象。热力学校正的影响不大,如果以气相构象稳定性排名为目标,则可以忽略。连续介质溶解的影响较强,尤其是在吉布斯自由能热力学校正的作用下,并导致构象能的扩散减小。团簇形成结合能在很大程度上取决于特定的振动热化学方法,传统谐波近似和修正比例刚性-谐波振荡器近似之间的差异达到 10 kcal mol-1。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

An influence of electronic structure theory method, thermodynamic and implicit solvation corrections on the organic carbonates conformational and binding energies

An influence of electronic structure theory method, thermodynamic and implicit solvation corrections on the organic carbonates conformational and binding energies

An impact of an electronic structure or force field method, gas-phase thermodynamic correction, and continuum solvation model on organic carbonate clusters (S)n conformational and binding energies is explored. None of the tested force field (GFN-FF, GAFF, MMFF94) and standard semiempirical methods (PM3, AM1, RM1, PM6, PM6-D3, PM6-D3H4, PM7) can reproduce reference RI-SCS-MP2 conformational energies. Tight-binding GFNn-xTB methods provide more realistic conformational energies which are accurate enough to discard the least stable conformers. The effect of thermodynamic correction is moderate and can be ignored if the gas phase conformational stability ranking is a goal. The influence of continuum solvation is stronger, especially if reinforced with the Gibbs free energy thermodynamic correction, and results in the reduced spread of conformational energies. The cluster formation binding energies strongly depend on a particular approach to vibrational thermochemistry with the difference between traditional harmonic and modified scaled rigid – harmonic oscillator approximations reaching 10 kcal mol−1.

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来源期刊
CiteScore
6.60
自引率
3.30%
发文量
247
审稿时长
1.7 months
期刊介绍: This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.
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