Heterogeneous Catalysts Tailored for Parahydrogen Induced Nuclear Spin Polarization

在化学系化学测量和成像项目的支持下，佛罗里达大学的Bowers和Hagelin-Weaver教授及其团队将联合收割机最先进的催化剂合成、表征和反应研究相结合，以确定和减轻仲氢诱导极化（PHIP）过程中减少成对氢化的过程。PHIP是用于灵敏度增强的核磁共振（NMR）光谱和磁共振成像的稳健且廉价的方法。除了潜在的生物医学应用外，PHIP是研究氢化催化的有力方法，在这项拟议的研究中获得的新见解可能会对氢化以外的催化反应领域产生重大影响。 学生将接受催化，反应器设计，材料表征和表面化学的跨学科培训。PI还建议通过与UF的CPET计划协调，为农村和城市学校的教师提供服务，这些学校为来自社会经济服务不足的家庭的50%或更多的学生提供教师招聘。拟议的外联工作将在前沿研究和中学STEM教育之间建立创新和富有成效的联系。拟议的研究旨在确定催化剂性质、活性和成对选择性之间的相关性。拟议的研究计划将是第一个将最先进的纳米颗粒制造策略与精密原子层沉积（ALD）结合起来的联合收割机。自旋密度矩阵理论将指导PHIP数据的解释。开发独特的PHIP NMR仪器是该项目的另一个关键要素。用氧化物和氧化物负载的金属颗粒获得的成对选择性目前限于几个百分比。使用工程氧化物负载的金属纳米颗粒催化剂获得显著更高的成对选择性将是该项目的变革性成果。这种低成对选择性的问题将通过基本的动力学和机理研究来解决。拟议的研究还旨在扩大可以通过这类催化剂超极化的靶标的种类。

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professors Bowers and Hagelin-Weaver and their groups at the University of Florida will combine state-of-the-art catalyst synthesis, characterization, and reaction studies to identify and mitigate the processes that reduce pairwise hydrogenation during Parahydrogen Induced Polarization (PHIP). PHIP is a robust and inexpensive method used for sensitivity enhanced nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging. In addition to potential biomedical utilization, PHIP is a powerful method for the study of hydrogenation catalysis and new insights gained during this proposed research may well have a major impact on the field of catalytic reactions, beyond hydrogenation. Students will receive interdisciplinary training in catalysis, reactor design, materials characterization, and surface chemistry. The PIs also propose to reach out to teachers from rural and urban schools serving 50% or more students from socio-economically underserved homes by coordinating with UF's CPET programs for teacher recruitment. The proposed outreach efforts will provide an innovative and productive linkage between cutting-edge research and secondary school STEM education.The proposed research seeks to identify correlations between catalyst properties, activity and pairwise selectivity. The proposed research plan will be the first to combine state-of-the art nanoparticle fabrication strategies with precision atomic layer deposition (ALD). Interpretation of PHIP data will be guided by spin density matrix theory. Development of unique PHIP NMR instrumentation is another key element of the project. Pairwise selectivities obtained with oxides and oxide supported metal particles are currently limited to a few percent. Attaining substantially higher pairwise selectivity using engineered oxide-supported metal nanoparticle catalysts would be a transformative outcome of the project. This low pairwise selectivity problem will be addressed through fundamental kinetic and mechanistic studies. The proposed studies also aim to broaden the variety of targets that can be hyperpolarized by this class of catalyst.