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：开发可转移的力场和蒙特卡洛算法以及对阶段和吸附平衡的应用，化学和生物技术工业中可持续过程的发展以及个人护理工业的新颖配方在个人护理和清洁工业中的新颖构想具有极高的商业和环境的重要性。分子水平的知识对于从基于试验和错误的方法转变为这些化学过程和配方的知识驱动设计至关重要。在此范围内，由Siepmann，Eggimann和Koenig领导的协作团队将开发准确的分子模型和有效的模拟算法，以推动分子模拟作为高效率性能预测的工具，并提供分子水平的见解，以实现相位和索取平衡。将解决与生物燃料生产和洗涤剂配方相关的特定应用。智力优点：模型发展。力场的陷阱（相位平衡的可转移电位）将在多个分辨率上扩展。 Trappecg（粗粒）将包括聚合物，沥青质和水； Trappe？UA（United-Atom）会添加硅氧烷和氯化乙烯基聚合物； Trappeeh（显式氢）将解决环境污染物和发酵抑制剂。可以通过对无机离子的Trappe盐和多孔沸石框架的trappe Zeo进行参数化来扩大适合预测模拟的系统和过程的范围。 Web界面将旨在提高其他研究小组的Trappe Force领域的可访问性。算法开发。将开发新的蒙特卡洛算法，可以改善相位转移的采样（例如，在液态液位平衡和溶液阶段的吸附等温线和吸附等温线）和微均质流体中的空间分布（例如，表面活性剂系统）。申请。使用Trappe力场的分子模拟将被用作工程工具，以预测各种复杂系统的热物理特性，从而增加了可用的实验数据库。这些模拟将为分子结构和组成如何确定宏观现象提供大量的微观级别洞察力。具体地，将进行模拟以调查（i）从发酵汤中基于溶剂的乙醇提取，ii）氧合溶液中的氧合和发酵抑制剂的吸附等温等温线，（iii）表面表面活性剂在界面和多电解剂（iiv）中的能力和（iv）的能力限制（iv），cosists of Organist and（IV）中的（iv）中的（iv）中的（iv）中的（iv）中的（iv）中的（iv）中的（iv）中的（iiv）中的（iiv）中的（iiv）中的（iiv）中的（IV）。在混合表面活性剂双层中。更广泛的影响：研究和教育的整合。由于发现的兴奋是学生学习的重要动机因素，因此Siepmann和Eggimann通常在其课堂教学中（涵盖来自物质世界的大一研讨会上的研究生统计学机制），将计算练习和分子模拟研究的局部效果进行了整合。西普曼（Siepmann）教授了三年级学生的动手科学课堂，并为UMN的工程和物理科学计划探索职业组织了围绕计算化学的全天活动。 Eggimann利用了一项积极的本科研究计划，以促进一般的科学素养和研究教学教学。人力资源的发展。该大学行业的伙伴关系独特地促进了研究生和博士后同事的教育和培训，允许与工业化学家进行广泛的互动，并与现实世界表面活性剂应用程序进行经验。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。拟议的计算调查提供的显微镜级别的理解将对设计改进的生物燃料和表面活性剂系统的分离过程非常有益。计算基础架构是通过自由分布的分布式分布的分子模拟包的开发，相关的Cyber​​tool和MCCC（用于复杂化学系统的Monte Carlo）的开发来提出计算基础架构。