CDS&E: Development and application of cluster-integral methods for dispersions and complex solutions

通过这一奖项，化学系的化学理论、模型和计算方法计划支持布法罗大学/纽约州立大学的David Kofke和Andrew Schultz开发一种分层的理论和计算方法来研究化学解决方案。化学溶液在天然和人造系统中普遍存在，它们的行为对许多技术应用至关重要，包括医疗保健、能源储存、环境保护以及食品和消费品。描述化学溶液的一种方法是通过溶质相互作用的层次结构，首先考虑溶质分子单独，然后成对，然后是三个、四个组，依此类推。这个层次结构中的每个级别都引入了关于混合物的新信息，因此人们可以通过对这些相互作用的适当分析来推断完整的行为。这种配方所需的量原则上可以从详细的分子考虑中计算出来，这是可取的，因为它导致了更好的预测和描述能力。然而，为了实际目的进行这些计算的手段还没有开发出来，因此整体方法的全部潜力相对来说还没有得到检验。这一方法的开发和基准是本研究项目的重点。该项目将研究生培训与外展活动相结合，并开发学习材料和计算机工具，使其他人能够从该项目的发展中受益。渗透维里方程构成了这项工作的理论框架。其研究目标是：(1)开发稳健和准确的方法，从分子模型计算渗透维里系数，至少达到5阶，同时建立扩展其覆盖范围的近似式；(2)研究硬凸粒子混合物的行为，特别是关注熵驱动的聚集和流体-液体相不稳定。使用这些簇积分方法的高通量筛选预计将产生至少5000个物种对的数据；(3)研究蛋白质在溶液中的结合，特别是考虑Crowder分子对这一行为的影响。

With this award, the the Chemical Theory, Models and Computational Methods Program in the Chemistry Division is supporting David Kofke and Andrew Schultz of the University at Buffalo/SUNY to develop a hierarchal theoretical and computational approach to studying chemical solutions. Chemical solutions are ubiquitous in natural and man-made systems, and their behavior is critical to many applications in technology, including healthcare, energy storage, environmental preservation, and food and consumer products. One approach to the description of chemical solutions is via a hierarchy of solute interactions, considering first the solute molecules individually, then taken in pairs, then groups of three, four, and so on. Each level in this hierarchy introduces new information about the mixture, such that one can infer the full behavior by proper analysis of these interactions. The quantities needed for this formulation can in principle be computed from detailed molecular considerations, which is desirable because it leads to greater predictive and descriptive capability. However, the means to perform these calculations for practical purposes have not been developed, so the full potential of the overall approach is relatively untested. Developing and benchmarking this approach is the focus of this research projects. The project integrates training of graduate students with outreach activities and development of learning materials and computer-based tools that permit others to benefit from the developments in this project.The osmotic virial equation forms the theoretical framework the work. The research objectives of are: (1) to develop robust and accurate methods for calculating osmotic virial coefficients up to at least 5th order, from a molecular model, while formulating approximants that extend their reach; (2) to examine behavior of mixtures of hard convex particles, focusing in particular on entropy-driven aggregation and fluid-fluid phase instability. High-throughput screening using these cluster-integral methods is anticipated to yield data for at least 5000 species pairs; (3) to investigate association of proteins in solution, considering in particular the effect of crowder molecules on this behavior.