Calculation of Diffusion Coefficients through Coarse-Grained Simulations Using the Automated-Fragmentation-Parametrization Method and the Recovery of Wilke-Chang Statistical Correlation

利用自动碎片化参数化方法通过粗粒化模拟计算扩散系数并恢复 Wilke-Chang 统计相关性

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Abstract

We introduce a model for the calculation of diffusion coefficients using dissipative particle dynamics coarse-grained molecular simulations. We validate the model on experimental diffusion data of small organics and drug-like molecules in water. The new model relies on our automated-fragmentation-parametrization protocol for cutting molecules into fragments, which are calibrated using the COSMO-RS thermodynamic model ( J. Chem. Inf. MODEL: 2016 , 56 ( 12 ), 2361 - 2377 , DOI: 10.1021/acs.jcim.6b00003 ). By simulations over the entire CULGI database of more than 11000 molecules, we recover the decades-old empirical Wilke-Chang correlation between diffusion coefficient and molar volume. We believe this is the first demonstration of the correlation by simulation or theory. From a comparison of simulated and experimental diffusion coefficients, we find that one full time unit of coarse-grained simulation equals 64 ± 13 ps real time.

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