Metal Organic Framework Materials for Efficient Separations of Liquid Mixtures

Sholl金属-有机框架（MOF）材料在其发展中处于新兴阶段，作为用于新应用的一大类纳米多孔材料，特别是在分离和催化中。该项目的中心主题是创建一个系统的计算和实验框架，用于理解MOF材料与氢键（极性）分子的相互作用。 PI提出了一个协同实验和建模的努力，定量测量水和醇（甲醇和乙醇）在MOFs的吸附和扩散性能。 分子吸附和扩散将直接使用最先进的气相重量分析法和高梯度强度脉冲场梯度核磁共振（PFG-NMR）方法与一系列选择的MOF系统地改变孔径和功能。 这些测量将显着扩大范围的定量实验信息，可在MOFs中的氢键分子的运输和吸附。 通过将我们的实验结果与一系列仔细的分子模拟直接比较，PI希望了解MOFs中氢键吸附和扩散的关键特征，并评估力场描述此类物质的能力。 除了对现有的MOF进行广泛的拟议工作外，PI还将研究混合沸石咪唑酯框架（ZIF）的性能，ZIF是格鲁吉亚理工学院最近开发的一类MOF材料。混合ZIF可以被制成具有连续可调的孔特征，并为优化分离中的材料性能创造新的机会。 PI将研究使用这种微调特性开发用于水-醇分离的高性能膜的可能性。 一个合理的框架的出现，以评估MOFs在液相分离将有长期的影响，在追求的应用MOFs在生物燃料加工和生物炼制业务。 近期的技术影响可能是成功选择和使用耐用的MOFs/ZIF，以创建与生物燃料加工相关的水-醇分离的高性能膜。 在更基本的层面上，这项工作将推进分离，多孔材料和计算化学工程社区的共同目标，克服高通量发现先进分离材料所固有的基本挑战。这项工作是潜在的变革，有助于提高多孔材料在化学分离中的作用，通过合理的设计方法。PI将通过对年轻和未来的工程师和科学家的职业生涯产生积极和可衡量的影响来追求这些预期的影响。PI将通过1-3年的精心设计和评估的学习经验，指导研究生，本科和高中水平的6-8名研究人员组成的多元化小组。这将包括博士论文项目，本科研究项目，以及与以STEM为重点的特许学校合作的高中生实习。 将研究成果转移到PI？纳米化学工程和分子模拟选修课将产生重大的教育影响。

1264874 ShollMetal-organic framework (MOF) materials are at an emerging stage in their development as a large class of nanoporous materials for new applications especially in separations and catalysis. The central theme of this project is to create a systematic computational and experimental framework for understanding the interactions of MOF materials with hydrogen-bonding (polar) molecules. The PIs propose a synergistic experimental and modeling effort to quantitatively measure the adsorption and diffusion properties of water and alcohols (methanol and ethanol) in MOFs. Molecular adsorption and diffusion will be measured directly using state-of-the-art vapor phase gravimetry and high-gradient-strength pulsed field gradient nuclear magnetic resonance (PFG-NMR) methods with a series of MOFs chosen to systematically vary pore size and functionality. These measurements will significantly expand the scope of quantitative experimental information that is available about hydrogen-bonding molecule transport and adsorption in MOFs. By directly comparing our experimental results with a careful series of molecular simulations, the PIs expect to understand the key features of hydrogen-bonded adsorption and diffusion in MOFs and assess the capability of force fields for describing such species. In addition to extensive proposed work with established MOFs, the PIs will also study the performance of hybrid zeolitic imidazolate framework (ZIFs), a class of MOF materials developed recently at Georgia Tech. Hybrid ZIFs can be made with continuously tunable pore characteristics and create new opportunities for optimizing material performance in separations. The PIs will examine the possibility of using this fine tuning property to develop high performance membranes for water-alcohol separations.Broader Impacts. The emergence of a rational framework for evaluating MOFs in liquid-phase separations will have long-term impact in the pursuit of applications for MOFs in biofuel processing and biorefinery operations. A nearer-term technological impact could be in the successful selection and use of robust MOFs/ZIFs to create high-performance membranes for water-alcohol separations relevant in biofuel processing. At a more fundamental level, this work will advance the shared goals of the separations, porous materials, and computational chemical engineering communities in overcoming basic challenges inherent in high-throughput discovery of advanced materials for separations. This works is potentially transformative in helping to enhance the role of porous materials in chemical separations through rational design methods. The PIs will pursue these desired impacts by creating a positive and measurable impact on the careers of young and prospective engineers and scientists. The PIs will mentor a diverse group of 6-8 researchers at graduate, undergraduate, and high school levels via carefully designed and assessed learning experiences over periods of 1-3 years. This will encompass PhD thesis projects, undergraduate research projects, and extended high-school student internships in collaboration with a STEM-focused charter school. The transfer of research findings into the PIs? elective courses on nanoscale chemical engineering and molecular modeling will have a significant educational impact.