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

摘要1159731 Eggimann，Becky L.Goali：合作研究：可转移力场和蒙特卡罗算法的发展以及在相和吸附平衡中的应用化学和生物技术工业中可持续工艺的发展以及个人护理和洗涤剂行业中新配方的开发具有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变为这些化学过程和配方的知识驱动的设计是必不可少的。为此，由Siepmann、Eggimann和Koenig领导的合作团队将开发准确的分子模型和高效的模拟算法，以推动分子模拟作为高保真性质预测的工具，并提供关于相和吸附平衡的分子水平的见解。与生物燃料生产和洗涤剂配方相关的具体应用将被讨论。TRAPPE(相平衡的可传递势)力场家族将在多个级别的分辨率下扩展。TraPPCG(粗粒)将包括聚合物、沥青质和水；Trappe？UA(联合原子)将添加硅氧烷和氯乙烯聚合物；TraPPEEH(显式氢气)将处理环境污染物和发酵抑制剂。通过对无机离子的Trappe盐和对多孔沸石骨架的Trappe Zeo的参数化，可以扩大适用于预测模拟的系统和过程的范围。将设计一个网络界面，以增加Trappe力场的可及性，供其他研究小组使用。算法开发。新的蒙特卡罗算法将被开发，它可以改进相转移(例如，在液-液平衡和溶液相的吸附等温线中)的采样和微非均相流体(例如，表面活性剂体系)中的空间分布。申请。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性质的工程工具，从而增加现有的实验数据库。这些模拟将提供丰富的微观层面的洞察，了解分子结构和组成如何决定宏观现象。具体地说，将进行模拟以研究(I)基于溶剂从发酵液中提取乙醇，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限制，以及(V)混合表面活性剂双层中的相共存。由于对发现的兴奋是学生学习的重要动机因素，Siepmann和Eggimann经常将分子模拟研究的计算练习和专题结果整合到他们的课堂教学中(从物质世界的新生研讨会到研究生级别的统计力学)。Siepmann教授了三年级学生的动手科学课堂，并为UMN的工程和物理科学探索职业计划组织了一整天的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促进普遍的科学素养和研究即教学的教学方法。人力资源开发。这一大学行业合作伙伴关系允许与工业化学家进行广泛的互动，并具有真实世界表面活性剂应用的经验，从而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，特别努力从传统上代表性不足的群体中招收这些学生。对科学和工程基础设施的影响。拟议的计算研究提供的微观层面的理解将对设计改进的生物燃料和表面活性剂体系的分离过程非常有益。计算基础设施的发展是由Trappe力场、相关的计算机工具和MCCCS(蒙特卡罗复杂化学系统)分子模拟程序包的开发推动的，这些程序是免费分布的。

Abstract1159731Eggimann, Becky L. GOALI: Collaborative Research: Development of transferable force fields and Monte Carlo algorithms and application to phase and sorption equilibriaThe 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 fieldsfor 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 affordedby 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.