Modelling Molecular Partitioning in Complex Media

拟议的研究侧重于开发新的理论模型和方法来估计环境中被认为对环境监测和管制政策工作具有重要意义的化学品的性质。我们特别关注缺乏坚实理论基础的有问题的领域，以开发新的、稳健的预测技术。例如：(1)在不同环境中改变其形态的化学品，其任何一种形态的性质不能充分代表分子的整体行为；(2)其他化学溶剂的复杂混合物中的化学品，该分子在任何一种溶剂中的性质不能充分代表分子的整体行为；(3)在土壤、泥浆或生物组织等成分未知的环境中的化学品，现有的性质估计方法不适用于这些化学品。 作为我们工作的基础，我们使用了最近发展起来的一种预测液体中化学物质性质的理论--COSMO-RS方法。这种方法以准确计算化学物质在松弛或完全溶解的环境中的结构为起点，以及化学物质的电子在化学主干上分布的相应方式。使用这些起点，该理论可以很好地预测水、空气或其他液体中会发现多少化学物质。 我们自己的工作将以下列方式解决上述问题领域：(1)改变其形式的化学品的详细化学成分将被纳入明确解释存在的各种形式的模型中；(2)存在于其他化学溶剂混合物中的化学品将通过模拟混合物或混合单个溶剂的性质的几种方法之一进行建模来处理；(3)未知组成环境将通过数学构建人工溶剂模型来表示，该模型的性质通过数学拟合使其与未知环境的性质相匹配。 这项工作的结果将有助于开发新的环境监测方法和技术，为政府制定属于上述类别的许多化学品和环境的监管政策提供信息。它们还将被现场和实验室的环境科学家用来准确测量此类化学物质的浓度和命运。最后，这些创新的延伸将带来新的方法，将人类和哺乳动物血液和组织中的生物分子作为全身命运模型的一部分进行理论化。

The proposed research focusses on the development of new theoretical models and methods for estimating the properties of chemicals in environments that are considered to be of importance in environmental monitoring and regulatory policy work. We are specifically focusing on the problematic areas that lack a solid theoretical foundation, to develop new, robust prediction techniques. Example areas are: (1) chemicals that change their form in different environments, for which the properties of any one of its forms do not adequately represent the molecule’s overall behaviour; (2) chemicals in complex mixtures of other chemical solvents for which the properties of that molecule in any one of the solvents do not adequately represent the molecule’s overall behaviour; (3) chemicals in environments of unknown composition such as soils, muds, or biological tissues, for which existing methods of property estimation are not usable. We use, as the basis for our work, a recently developed theory for the prediction of the properties of chemicals in liquids, the COSMO-RS method. This method uses as its starting point an accurate calculation of the chemical’s structure in a relaxed or fully solvated environment, along with the corresponding way in which the chemical’s electrons distribute themselves over the chemical backbone. Using these starting points, the theory can predict how much of a chemical will be found in water, air, or other liquids to a good level of accuracy. Our own work will address the above problem areas in the following ways: (1) the detailed chemistry of chemicals that change their form will be incorporated into models that explicitly account for the various forms present (2) chemicals present in mixtures of other chemical solvents will be treated by modelling the solvent mixture by one of several methods that either mimic the mixture or blend the properties of the individual solvents and (3) unknown composition environments will be represented by mathematically constructing an artificial solvent model whose properties are matched by mathematically fitting them to the properties of the unknown environment. The results of this work will aid in the development of new environmental monitoring approaches and techniques that will inform government regulatory policy of many chemicals and environments that fall into the categories noted above. They will also be used by environmental scientists in the field and laboratory to accurately measure concentrations and fates of such chemicals. Finally, extensions of these innovations will lead to new ways to theorize biomolecules in human and mammalian blood and tissues as part of whole-body fate models.