GOALI: Development of Transferable Force Fields for Phase Equilibria and Simulation Studies of Microheterogeneous Fluids

目标：相平衡可转移力场的开发和微非均质流体的模拟研究

• 批准号: 0138393
• 负责人: Joern Ilja Siepmann
• 金额: $ 28.23万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2002
• 资助国家: 美国
• 起止时间: 2002-06-01 至 2006-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0138393&HistoricalAwards=false
• 关键词: GOALI; Development; Transferable; Force; Fields

AbstractCTS-0138393Siepmann, Joern I.University of Minnesota - Twin CitiesAccurate knowledge of the phase equilibria and other thermophysical properties of complex fluid mixtures are of enormous fundamental and practical importance. The success of molecular simulation in predicting thermophysical properties an in advancing our understanding of the relationship between molecular architecture and macroscopic observable depends on the availability of efficient simulation algorithms and accurate force fields.The goals of the research are to continue the development of three levels of transferable force fields and of biased Monte Carlo methods. The first-level force field, called TraPPE-UA (transferable potentials for phase equilibria-united atom), employs the united-atom representation for alkyl segments and simple Lennar -Jones an Coulombic terms. In the second level, called TraPPE -EH (explicit hydrogen), all atoms including alkyl group hydrogens and some lone-pair electron and bond-center sites are treated explicitly. In the third-level, called TraPPE-pol (polarizable), both the van der Waals and electrostatic interactions can respond to changes in the environment. Whereas the first level is designed for simplicity and computational efficiency with good accuracy, the second level is aimed at improved accuracy for mixtures of non-polar or apolar non-hydrogen-bonding compounds. The third level is directed solely at the highest possible level of accuracy and transferability. These transferable force fields will encompass linear, branched, and cyclic alkanes, alkenes, alkynes, alkylbenzenes, alcohols, ethers, ketones, aldehydes, esters, carboxylic acids amines, amides, nitriles, thiols, sulfides, heterocycles, perfluorinated alkanes, and last, but not least, water. In addition to the force field development, this proposal also addresses novel simulation algorithms which are targeted at efficient simulations of solid-fluid equilibria, spatially heterogeneous mixtures, and hydrogen-bonded networks.Molecular simulations using the transferable force fields will be employed as engineering tool topredict thermophysical properties of a variety of systems, thereby adding to the available experimental database. The simulations will also provide a wealth of microscopic-level information for complex chemical systems, thereby giving new physical insight into how molecular architecture and composition determine macroscopic phenomena. In particular, simulations will be carried out to investigate the association of alcohols in non-polar solvents, the influence of entrainers on structure and solubility in supercritical fluids, the effect of pressurization on gas-expanded liquids, the solute partitioning between water and octan-1-ol at elevated temperatures and pressures, the structures of minimum and maximum boiling azeotropic mixtures, the liquid-liquid equilibria of alcohol/water mixtures, the partial solubilities of drugs and their sodium derivatives, and the influence of solvents on the stability of polymorphs and on solvate formation.This project will profit from extensive collaboration of a close university-industry team consistingof the PI and Dr. Sami Karaborni of Merck Research Laboratories.

Abstractcts -0138393Siepmann，Joern I.明尼苏达州的大学 - 双城市对相位平衡的知识和复杂液体混合物的其他热物理特性具有巨大的基本和实际重要性。 分子模拟在预测热物理特性方面的成功促进了我们对分子结构与可观察的宏观构建之间的关系的理解取决于有效的模拟算法和准确的力场的可用性。 一级力场，称为trappe-ua（相位平衡的原子的可转移电位），采用烷基段的联合原子代表，而简单的lennar -Jones则是库仑的术语。 在第二层，称为trappe -eh（显式氢），所有原子在内，包括烷基氢和某些孤对电子和键中心位点，都可以明确处理。 在称为trappe-pol（可极化）的第三级中，范德华和静电相互作用都可以响应环境的变化。 虽然第一级是为了简单和计算效率而设计的，但第二级旨在提高非极性或非极性非氢键键化化合物混合物的精度。 第三级仅针对最高的准确性和可传递性水平。 这些可转移的力场将涵盖线性，分支和环状烷烃，烷烃，炔烃，烷基苯苯甲苯，酒精，乙醇，醚，酮，酮，酯，酯，羧酸，羧酸胺，胺，胺，氮，硫化物，硫化物，硫化物，硫化物，硫化物，硫化物，水孔，最小孔，终极孔，且始终渗透且局部孔，且近距离群体群孔，且近距离渗透且近距离孔，且近距离群体，且近距离渗透，且近距离群体，且近距离渗透效果层孔，且近距离渗透。 除了力场开发外，该提案还解决了针对有效模拟固体氟平衡，空间异质混合物和氢键网络的新型模拟算法。使用可转移力领域的氢分子模拟将用于工程工具工具的热物体，以添加各种系统，以添加各种系统，以添加可转移力领域。 这些仿真还将为复杂的化学系统提供大量的显微镜信息，从而为分子结构和组成如何确定宏观现象提供了新的物理见解。 In particular, simulations will be carried out to investigate the association of alcohols in non-polar solvents, the influence of entrainers on structure and solubility in supercritical fluids, the effect of pressurization on gas-expanded liquids, the solute partitioning between water and octan-1-ol at elevated temperatures and pressures, the structures of minimum and maximum boiling azeotropic mixtures, the liquid-liquid equilibria of alcohol/water混合物，药物及其钠衍生物的部分溶解度以及溶剂对多晶型物和溶剂化物组的稳定性的影响。该项目将从PI和Merck Research Laboratories的PI和Sami Karaborni博士组成的密切大学工作团队的广泛合作中获利。