Molecular Modeling of Environmentally Benign Solute-Solvent Systems

McCabe，Clare MColorado矿业学院“环境友好的溶质-溶剂系统的分子模型”由于目前的溶剂已被禁止或不鼓励使用，溶剂替换-即用环境可接受的溶剂取代反应、分离和溶解/清洗操作中的危险和/或致癌溶剂-是将现有工艺转变为环境友好工艺的关键方法之一。在追求环境友好的过程中，包括超临界二氧化碳和离子液体在内的近代溶剂的应用显示出巨大的工业应用潜力，我们建议的研究重点正是这些流体。未来的重点是设计环境友好的过程-无论是通过溶剂替代实现的，还是通过开发全新的环境友好的化学过程实现的-与迫切需要一种准确的综合方法来计算与这些溶剂的应用相关的操作条件下含有新型溶剂的混合物的热力学性质(特别是相平衡)。对于环境友好过程中预计会遇到的各种条件和体系，预测热力学性质(包括相平衡)的方法应该是健壮、快速和通用的。为了解决这一需求，PI建议开展一项持续的研究计划，其目标是应用分子理论和模拟来开发、修改和部署基于分子水平统计缔合流体理论(SAFT)与其他分子建模技术相结合的基于预测的分子方法学。PI相信，由此产生的方法将成为环境友好型工艺设计的首选建模平台。加强SAFT在与电子商务系统相关的关键领域的预测能力的理论发展--促进潜在模型开发和测试的从头方法，以及提供严格理论测试和帮助潜在模型开发的计算机模拟--的结合将使真正的预测平台得以实现。为了实现这一目标，与电子商务进程相关的两个广泛的应用领域将是国际和平研究所研究活动的长期重点。第一个领域是通过将这些体系中的基本分子相互作用纳入理论方法来精确模拟极性聚合物-溶剂和共聚-溶剂体系。其次，PI将致力于发展急需的模型和分子理论来描述离子液体及其混合物的热力学性质。在这项建议中，国际和平倡议将专注于这两个领域中的第一个领域。拟议的研究是实现国际和平倡议长期目标的第一步。从该项目中吸取的经验教训将促进在其他应用领域取得类似进展。在整个项目中，将保持与行业和实验小组的密切联系，这将为学生提供体验研究的理论和实验方面的机会，验证我们的方法和模型的手段，并就行业在采用对环境无害的现有和新工艺替代方案时面临的关键问题提供指导。这项研究的结果将被纳入到PI正在开发的基于主动学习的分子建模课程中。这门课程将适合研究生和本科生，这将确保CSM的学生将接触和参与分子建模和EB过程的分子热力学的前沿。将通过研究项目大力鼓励本科生参与该项目，并通过国际社会参与CSM与科学相关的学位项目积极招募妇女和少数族裔，该项目为这些代表性不足的群体的本科生提供指导研究项目。

McCabe, Clare MColorado School of Mines"Molecular Modeling of Environmentally Benign Solute-Solvent Systems" As current solvents have become banned or discouraged from use, solvent replacement - i.e., replacing a hazardous and/or carcinogenic solvent in reaction, separation, and dissolution/cleaning operations with an environmentally acceptable one - is one of the key methods for turning an existing process into an environmentally benign one. In the pursuit of environmentally benign processes, the application of neoteric solvents, including supercritical carbon dioxide and ionic liquids, show enormous potential for industrial application and it is these fluids that we focus our proposed research on.The future focus on the design of environmentally benign processes - whether achieved by solvent replacement or by the development of fundamentally new environmentally benign chemical processes - parallels a crucial emerging need for an accurate comprehensive methodology for calculating the thermodynamic properties (especially phase equilibria) of mixtures containing novel solvents at operating conditions relevant to the application of these solvents. For the wide range of conditions and systems expected to be encountered in environmentally benign processes, the method for predicting thermodynamic properties (including phase equilibria) should be robust, rapid and versatile. The PI proposes to address this need by undertaking a sustained research program whose goal is to apply molecular theory and simulation to the development, modification and deployment of a predictive molecular-based methodology based on the molecular-level statistical associating fluid theory (SAFT) integrated with other molecular modeling techniques. The PI believes that the resulting methodology will be the modeling platform of choice for the design of environmentally benign processes. A combination of theoretical developments to enhance the predictive capabilities of SAFT in key areas relevant to EB systems - ab initio methods to facilitate potential model development and testing, and computer simulations to provide both a rigorous test of the theory and aid in potential model development - will enable a true predictive platform to be realized. In pursuit of this goal two broad application areas relevant to EB processes will be the long-term focus of the PI's research activities. The first area is the accurate modeling of polar polymer-solvent, and co-polymer-solvent systems through the incorporation of the underlying molecular interactions in these systems into the theoretical approach. Secondly the PI will concentrate efforts on developing much need models and molecular theory for describing the thermodynamic properties of ionic liquids and their mixtures. In this proposal, the PI will focus on the first of these two areas.The proposed research is the first step towards achieving the PI's long-term goals. The lessons learned from this project will facilitate similar advances in other application areas. Strong ties with industry and experimental groups will be maintained throughout the project which will provide students with the opportunity to experience both the theoretical and experimental sides of research, a means to validate our methods and models, and provide guidance towards key problems faced by industry in adopting environmentally benign alternatives to existing, and new processes. The results of this research will be incorporated into an active-learning-based molecular modeling course, under development by the PI. The course will be suitable for both graduates and undergraduate students, which will ensure that students at CSM will be exposed to and participate in the frontiers of molecular modeling and the molecular thermodynamics of EB processes. Undergraduate participation in the project will be strongly encouraged through research projects and women and minorities actively recruited through the PI's participation in the Science Related Degrees project at CSM, which offers mentored research projects for undergraduate students in these underrepresented groups.