Poly(ethylene oxide) and Water: Simulations and Modeling of Solution Properties, Phase Behavior, Partitioning and Particle Interactions

0076306史密斯该补助金由化学和材料研究部门的理论化学和材料理论计划共同资助。 聚（环氧乙烷）（PEO），也称为聚（乙二醇），用于从减阻到药物递送的多种水溶液应用中。 此外，PEO溶液已被广泛研究，其本身具有根本意义，并且在更好地理解聚合物水溶液的努力中充当模型系统。 实验和建模研究导致了宝贵的洞察PEO解决方案的行为。 然而，这些解决方案的许多最有趣的特性导致其广泛的应用范围，例如构象，疏水相互作用，相行为，盐的影响以及聚合物与颗粒和蛋白质的相互作用，该研究的主要目标是通过协调模拟来提高对聚合物水溶液行为的理解，PEO解决方案的建模研究，开发和传播进行这些研究所需的计算算法和工具，并使本科生熟悉分子建模的能力和实用性。 原子分子动力学模拟研究将进行，以调查的构象，结构，热力学和动力学性质的PEO水溶液。 额外的模拟旨在专门了解PEO溶液的相行为，包括分子量和压力的影响，以及聚合物构象，水结构和醚-水氢键的作用，将进行。 最后，模拟研究的PEO解决方案与模型纳米粒子和蛋白质的相互作用将进行，旨在获得更好地了解聚合物介导的颗粒之间的耗尽吸引力，以及竞争性水合作用和疏水聚合物-颗粒相互作用的作用。 要实现这些科学目标，需要能够在广泛的长度范围内解决溶液的性质。 将创建一个力场开发工具包，通过精确的经典原子势函数的参数化，将电子结构水平与原子水平联系起来。 反过来，PEO溶液的原子分子动力学模拟的详细结果将作为聚合物溶液和聚合物与颗粒相互作用的液态理论模型的输入，潜在地扩展原子研究的长度尺度，以及允许远超出分子动力学模拟直接访问的参数空间的调查。提高对PEO解决方案的理解。 这些努力将大大增加的水溶液的行为的整体理解，合成和生物，以及一般的聚合物溶液，特别是在交叉浓度制度和在较高的浓度，那里是一个缺乏模拟研究。 所提出的模拟，如力场开发工具包和方法，用于确定自由能和聚合物溶液中的相平衡的计算工具和算法，将广泛有益于模拟社区。 目前用于研究生教学以及研究生和本科生水平研究的分子动力学模拟工具将发展成为本科生课程的工具，并将包括材料模拟和属性预测模块，旨在为本科生提供计算材料科学的实践经验。 该补助金分别由化学和材料研究部的理论化学和材料理论计划共同资助。 聚（环氧乙烷）（PEO），也称为聚（乙二醇），用于从减阻到药物递送的多种水溶液应用中。 此外，PEO溶液已被广泛研究，其本身具有根本意义，并且在更好地理解聚合物水溶液的努力中充当模型系统。 实验和建模研究导致了宝贵的洞察PEO解决方案的行为。 然而，这些解决方案的许多最有趣的特性导致其广泛的应用范围，例如构象，疏水相互作用，相行为，盐的影响以及聚合物与颗粒和蛋白质的相互作用，该研究的主要目标是通过协调模拟来提高对聚合物水溶液行为的理解，PEO解决方案的建模研究，开发和传播进行这些研究所需的计算算法和工具，并使本科生熟悉分子建模的能力和实用性。***

0076306SmithThis grant is funded jointly by the Theoretical Chemistry and Materials Theory Programs in the Divisions of Chemistry and Materials Research respectively. Poly(ethylene oxide) (PEO), also referred to as poly(ethylene glycol), is used in a multitude of aqueous solution applications ranging from drag reduction to drug delivery. In addition, PEO solutions have been widely studied, being themselves of fundamental interest as well as serving as model systems in efforts to better understand aqueous polymer solutions. Experimental and modeling studies have resulted in valuable insight into the behavior of PEO solutions. However, many of the most interesting characteristics of these solutions responsible for their broad scope of applications, such as conformations, hydrophobic interactions, phase behavior, the influence of salts, and the interactions of the polymer with particles and proteins, remain at best poorly understood.The principal goals of the research are to gain improved understanding of the behavior of aqueous polymer solutions through coordinated simulation and modeling studies of PEO solutions, to develop and disseminate the computational algorithms and tools required to carry out these studies, and to familiarize undergraduate students students with the power and utility of molecular modeling. Atomistic molecular dynamics simulation studies will be carried out in order to investigate the conformational, structural, thermodynamics and dynamic properties of aqueous PEO solutions. Additional simulations aimed specifically at understanding the phase behavior of PEO solutions, including the influence of molecular weight and pressure as well as the role of polymer conformations, water structure, and ether-water hydrogen bonding, will be performed. Finally, simulation studies of the interactions of PEO solutions with model nanoparticles and proteins will be carried out, aimed at gaining a better understanding of polymer mediated depletion attraction between particles as well as the roles of competitive hydration and hydrophobic polymer-particle interactions. Acheiving these scientific goals requires the capability of addressing solution properties over a wide range of length scales. A force field development toolkit will be created to link the electronic structure level to the atomistic level through parametrization of accurate classical atomistic potential functions. In turn, the detailed results of atomistic molecular dynamics simulations of PEO solutions will serve as input into liquid state theory models for polymer solutions and interactions of polymers with particles, potentially extending the length scale of the atomistic studies as well as allowing investigation of parameter space well beyond that directly accessible by molecular dynamics simulations.These studies have important ramifications beyond the benefits provided by an improved understanding of PEO solutions. These efforts will add significantly to the overall understanding of the behavior of aqueous solutions, both synthetic and biological, as well as that of polymer solutions in general, particularly in crossover concentration regimes and at higher concentrations where there is a paucity of simulation studies. The computational tools and algorithms developed for the proposed simulations, such as the force field development toolkit and methods for determining free energies and phase equilibrium in polymer solutions, will be widely beneficial to the simulation community. Molecular dynamics simulations tools, currently used for graduate teaching as well as graduate and undergraduate level research, will be developed into tools for undergraduate coursework and will include materials simulation and property prediction modules designed to give undergraduate students hands-on experience with computational materials science.%%% This grant is funded jointly by the Theoretical Chemistry and Materials Theory Programs in the Divisions of Chemistry and Materials Research respectively. Poly(ethylene oxide) (PEO), also referred to as poly(ethylene glycol), is used in a multitude of aqueous solution applications ranging from drag reduction to drug delivery. In addition, PEO solutions have been widely studied, being themselves of fundamental interest as well as serving as model systems in efforts to better understand aqueous polymer solutions. Experimental and modeling studies have resulted in valuable insight into the behavior of PEO solutions. However, many of the most interesting characteristics of these solutions responsible for their broad scope of applications, such as conformations, hydrophobic interactions, phase behavior, the influence of salts, and the interactions of the polymer with particles and proteins, remain at best poorly understood.The principal goals of the research are to gain improved understanding of the behavior of aqueous polymer solutions through coordinated simulation and modeling studies of PEO solutions, to develop and disseminate the computational algorithms and tools required to carry out these studies, and to familiarize undergraduate students students with the power and utility of molecular modeling. ***