Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, United States.
Department of Geosciences, Princeton University, Princeton, New Jersey 08544, United States.
Environ Sci Technol. 2023 Apr 18;57(15):6296-6308. doi: 10.1021/acs.est.3c00267. Epub 2023 Apr 4.
The tendency of organic contaminants (OCs) to partition between different phases is a key set of properties that underlie their human and ecological health impacts and the success of remediation efforts. A significant challenge associated with these efforts is the need for accurate partitioning data for an ever-expanding list of OCs and breakdown products. All-atom molecular dynamics (MD) simulations have the potential to help generate these data, but existing studies have applied these techniques only to a limited variety of OCs. Here, we use established MD simulation approaches to examine the partitioning of 82 OCs, including many compounds of critical concern, at the water-air interface. Our predictions of the Henry's law constant () and interfacial adsorption coefficients (, ) correlate strongly with experimental results, indicating that MD simulations can be used to predict , , and values with mean absolute deviations of 1.1, 0.3, and 0.3 logarithmic units after correcting for systematic bias, respectively. A library of MD simulation input files for the examined OCs is provided to facilitate future investigations of the partitioning of these compounds in the presence of other phases.
有机污染物（OCs）在不同相之间分配的趋势是其对人类和生态健康影响以及修复工作成功的关键属性。这些努力面临的一个重大挑战是需要为不断扩大的 OCs 和分解产物清单提供准确的分配数据。全原子分子动力学（MD）模拟有可能帮助生成这些数据，但现有研究仅将这些技术应用于有限种类的 OCs。在这里，我们使用成熟的 MD 模拟方法来研究 82 种 OCs 在水-气界面处的分配情况，其中包括许多具有重要关注价值的化合物。我们对亨利定律常数（Henry's law constant）（）和界面吸附系数（adsorption coefficients）（）的预测与实验结果密切相关，这表明 MD 模拟可用于预测、和值，经系统偏差校正后，平均绝对偏差分别为 1.1、0.3 和 0.3 个对数单位。提供了一个针对所研究的 OCs 的 MD 模拟输入文件库，以方便未来研究这些化合物在其他相存在下的分配情况。
