Manchester Institute of Biotechnology, The University of Manchester, 131 Princess Street, Manchester, M1 7DN, UK.
School of Chemistry, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK.
J Comput Aided Mol Des. 2021 Jul;35(7):831-840. doi: 10.1007/s10822-021-00401-w. Epub 2021 Jul 10.
Partition coefficients quantify a molecule's distribution between two immiscible liquid phases. While there are many methods to compute them, there is not yet a method based on the free energy of each system in terms of energy and entropy, where entropy depends on the probability distribution of all quantum states of the system. Here we test a method in this class called Energy Entropy Multiscale Cell Correlation (EE-MCC) for the calculation of octanol-water logP values for 22 N-acyl sulfonamides in the SAMPL7 Physical Properties Challenge (Statistical Assessment of the Modelling of Proteins and Ligands). EE-MCC logP values have a mean error of 1.8 logP units versus experiment and a standard error of the mean of 1.0 logP units for three separate calculations. These errors are primarily due to getting sufficiently converged energies to give accurate differences of large numbers, particularly for the large-molecule solvent octanol. However, this is also an issue for entropy, and approximations in the force field and MCC theory also contribute to the error. Unique to MCC is that it explains the entropy contributions over all the degrees of freedom of all molecules in the system. A gain in orientational entropy of water is the main favourable entropic contribution, supported by small gains in solute vibrational and orientational entropy but offset by unfavourable changes in the orientational entropy of octanol, the vibrational entropy of both solvents, and the positional and conformational entropy of the solute.
分配系数量化了分子在两种不混溶液相之间的分布。虽然有许多方法可以计算分配系数,但目前还没有一种方法是基于每个系统的能量和熵的自由能,其中熵取决于系统所有量子态的概率分布。在这里,我们测试了一种称为能量熵多尺度细胞相关(EE-MCC)的方法,用于计算 SAMPL7 物理性质挑战(蛋白质和配体建模的统计评估)中 22 种 N-酰基磺酰胺的辛醇-水 logP 值。EE-MCC logP 值的平均误差为 1.8 logP 单位,相对于实验,三个独立计算的均方根误差为 1.0 logP 单位。这些误差主要是由于获得足够收敛的能量以给出大数的准确差异,特别是对于大分子溶剂辛醇。然而,这也是熵的一个问题,力场和 MCC 理论中的近似也会导致误差。MCC 特有的是,它解释了系统中所有分子的所有自由度的熵贡献。水分子的取向熵增加是主要的有利熵贡献,这得到了溶质振动和取向熵的小幅度增加的支持,但被辛醇取向熵、两种溶剂的振动熵以及溶质的位置和构象熵的不利变化所抵消。