RUI: Probing adsorbate interactions in metal-organic frameworks using site selective spectroscopy

在这个由化学部门化学结构、动力学和机理a项目资助的项目中，Oberlin学院的Stephen FitzGerald教授研究了用于储存和分离氢气不同同位素的新型多孔材料。缺乏可行的车载氢存储被视为燃料电池动力汽车发展的主要障碍。就核、医学和科学研究界广泛使用的氢同位素而言，正是同位素分离的困难极大地增加了成本并抑制了其更多的使用。为了应对这些挑战，该项目专注于使用红外和质谱相结合的方法来了解金属有机框架孔隙内吸附质分子的量子行为。温度和浓度相关光谱揭示了位置特定的焓和吸附熵区分不同的结合机制，并利用零点能量差异引起的量子筛分效应建立了同位素分离的可行性。这些信息用于指导国家实验室和研究型大学的合作者制造具有优化气体储存和分离性能的新材料。除了氢动力汽车和更高效的气体分离技术带来的社会效益外，这项工作还通过指导本科生与首席研究员一对一的工作，产生了更广泛的影响。这些学生在欧柏林学院进行所有的研究，同时获得与研究型大学和国家实验室更大合作的经验。

In this project funded by the Chemical Structure, Dynamics and Mechanisms-A program of the Chemistry Division, Professor Stephen FitzGerald of Oberlin College investigates novel porous materials for both storing and separating the different isotopes of hydrogen gas. The lack of viable, on-board hydrogen storage is seen as the major impediment to the development of fuel cell powered automobiles. In the case of hydrogen isotopes, used extensively by the nuclear, medical, and scientific research communities, it is the difficulty of isotope separation that dramatically increases cost and inhibits greater use. To meet these challenges this project focuses on using a combination of infrared and mass spectroscopy to understand the quantum behavior of adsorbate molecules confined within the pores of metal-organic frameworks. Temperature and concentration dependent spectra revealing site-specific enthalpy and entropy of adsorption differentiate between different binding mechanisms and establish the viability of isotopic separation using quantum sieving effects arising from differences in zero-point energy. This information is used to guide collaborators at national laboratories and research universities in the fabrication of new materials with optimized properties for gas storage and separation. Beyond the societal benefits of hydrogen powered cars and more efficient gas separation techniques, this work has a broader impact through mentoring of the undergraduate students working one on one with the principal investigator. These students perform all the research at Oberlin College, while gaining experience of a larger collaboration of research universities and national laboratories.