GOALI: RUI: Collaborative Research: Development of Transferable Force Fields and Monte Carlo Algorithms and Application to Phase and Sorption Equilibria

目标：RUI：协作研究：可转移力场和蒙特卡罗算法的开发以及在相和吸附平衡中的应用

• 批准号: 1159837
• 负责人: Joern Ilja Siepmann
• 金额: $ 30万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-04-15 至 2015-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1159837&HistoricalAwards=false
• 关键词: GOALI; RUI; Collaborative; Research; Development

Abstract 1159837 Siepmann, Joern IljaGOALI: Collaborative Research: Development of transferable force fields and Monte Carlo algorithms and application to phase and sorption equilibria The development of sustainable processes in the chemical and biotechnology industries and of novel formulations in the personal care and detergent industries is of tremendous commercial and environmental importance. Molecular-level knowledge is essential for moving from trial-and-error based approaches to knowledge-driven design of these chemical processes and formulations. To this extent, accurate molecular models and efficient simulation algorithms will be developed by a collaborative team led by Siepmann, Eggimann, and Koenig to advance molecular simulation as a tool for high-fidelity property prediction and for providing molecular-level insights on phase and sorption equilibria. Specific applications relevant for biofuel production and detergent formulations will be addressed. Intellectual Merit: Model Development. The TraPPE (transferable potentials for phase equilibria) family of force fields will be extended at multiple levels of resolution. TraPPECG (coarse-grain) will include polymers, asphaltenes, and water; TraPPE?UA (united-atom) will add siloxane and vinyl chloride polymers; TraPPEEH (explicit-hydrogen) will address environmental pollutants and fermentation inhibitors. The range of systems and processes amenable to predictive simulations will be enlarged through the parameterization of TraPPE salt for inorganic ions and TraPPE zeo for porous zeolite frameworks. A web interface will be designed to increase the accessibility of the TraPPE force fields for other research groups. Algorithm Development. Novel Monte Carlo algorithms will be developed that can improve the sampling of phase transfers (e.g., in liquid-liquid equilibria and sorption isotherms from solution phases) and spatial distributions in microheterogeneous fluids (e.g,, surfactant systems). Applications. Molecular simulations using the TraPPE force fields will be employed as an engineering tool to predict thermophysical properties of a variety of complex systems, thereby adding to the available experimental database. The simulations will provide a wealth of microscopic-level insight into how molecular architecture and composition determine macroscopic phenomena. Specifically, simulations will be carried out to investigate (i) the solvent-based extraction of ethanol from fermentation broths, ii) the sorption isotherms of oxygenates and fermentation inhibitors from aqueous solution, (iii) the adsorption of surfactants at interfaces and to polyelectrolytes, (iv) the capacity limit of organics in micellar surfactants, and (v) the phase coexistence in mixed surfactant bilayers. Broader Impacts: Integration of Research and Education. Because the excitement of discovery is a significant motivating factor in student learning, computational exercises and topical results from molecular simulation research are routinely integrated by Siepmann and Eggimann in their classroom teaching (spanning from of a freshman seminar on the material world to graduate-level statistical mechanics). Hands-on science classroom for third graders have been taught by Siepmann and a full day of activities centered around computational chemistry is organized for UMN's Exploring Careers in Engineering and Physical Sciences Program. An active undergraduate research program is leveraged by Eggimann to promote general scientific literacy and research-as-teaching pedagogies. Development of Human Resources. This university industry partnership uniquely advances the education and training of the graduate students and postdoctoral associates by allowing for extensive interactions with industrial chemists and experience with real-world surfactant applications. Additionally, this project will foster the participation of undergraduate and high school students, with special efforts made to recruit these students from traditionally underrepresented groups. Impact on Science and Engineering Infrastructure. The microscopic-level understanding afforded by the proposed computational investigations will be highly beneficial for the design of improved separation processes for biofuels and surfactant systems. The computing infrastructure is advanced by the development of the TraPPE force fields, the associated cybertool, and the MCCCS (Monte Carlo for Complex Chemical Systems) molecular simulation package, which are freely distributed.

摘要 1159837 Siepmann、Joern IljaGOALI：合作研究：可转移力场和蒙特卡罗算法的开发以及在相和吸附平衡中的应用化学和生物技术行业的可持续工艺以及个人护理和洗涤剂行业的新型配方的开发非常重要巨大的商业和环境重要性。分子水平的知识对于从基于试错的方法转向知识驱动的化学工艺和配方设计至关重要。在这个意义上，由 Siepmann、Eggimann 和 Koenig 领导的协作团队将开发准确的分子模型和高效的模拟算法，以推进分子模拟作为高保真性质预测和提供有关相和吸附的分子水平见解的工具平衡。将讨论与生物燃料生产和洗涤剂配方相关的具体应用。智力优势：模型开发。 TraPPE（相平衡的可转移势）力场系列将在多个分辨率级别上扩展。 TraPPECG（粗粒）将包括聚合物、沥青质和水； TraPPE?UA（联合原子）会添加硅氧烷和氯乙烯聚合物； TraPPEEH（显式氢）将解决环境污染物和发酵抑制剂的问题。通过无机离子的 TraPPE 盐和多孔沸石框架的 TraPPE zeo 的参数化，将扩大适合预测模拟的系统和过程的范围。将设计一个网络界面，以提高其他研究小组对 TraPPE 力场的可访问性。算法开发。将开发新的蒙特卡罗算法，可以改进相转移的采样（例如，液-液平衡和溶液相的吸附等温线）和微异质流体（例如表面活性剂系统）的空间分布。应用。使用 TraPPE 力场的分子模拟将被用作预测各种复杂系统的热物理特性的工程工具，从而添加到可用的实验数据库中。这些模拟将为分子结构和组成如何决定宏观现象提供丰富的微观层面的见解。具体来说，将进行模拟以研究（i）从发酵液中以溶剂为基础的乙醇提取，ii）含氧物和发酵抑制剂从水溶液中的吸附等温线，（iii）表面活性剂在界面和聚电解质上的吸附， (iv) 胶束表面活性剂中有机物的容量极限，以及 (v) 混合表面活性剂双层中的相共存。更广泛的影响：研究与教育的整合。由于发现的兴奋感是学生学习的重要激励因素，Siepmann 和 Eggimann 经常将计算练习和分子模拟研究的主题结果整合到课堂教学中（从新生的物质世界研讨会到研究生水平的统计）力学）。西普曼为三年级学生开设了实践科学课堂，并为UMN的工程和物理科学职业探索项目组织了一整天以计算化学为中心的活动。 Eggimann 利用积极的本科生研究计划来提高普通科学素养和研究教学法。人力资源开发。这种大学行业合作伙伴关系通过允许与工业化学家的广泛互动以及实际表面活性剂应用的经验，独特地促进了研究生和博士后的教育和培训。此外，该项目将促进本科生和高中生的参与，并特别努力从传统上代表性不足的群体中招募这些学生。对科学和工程基础设施的影响。所提出的计算研究提供的微观层面的理解将非常有利于生物燃料和表面活性剂系统的改进分离过程的设计。通过免费分发的 TraPPE 力场、相关网络工具和 MCCCS（复杂化学系统蒙特卡罗）分子模拟包的开发，计算基础设施得到了进步。