Gated Molecular Encapsulation and Reactivity

化学结构、动力学和机制项目支持俄亥俄州立大学Jovica Badjic教授的一个项目，该项目将研究一系列新的动态受体-门控分子筐的效用，用于开发有关在受限环境中有效控制化学反应性的概念。利用计算和实验工具，研究人员旨在了解和量化多个（不止一个）分子进出分子筐的运输，并提出两种新的自组装和折叠框架，用于控制宿主的动力学，从而控制分子封装的动力学。他们还旨在获得手性分子进入/退出门控分子宿主的识别动力学控制。通过门控调节这种动力学分辨对于开发利用人工宿主识别立体异构体化合物的方法和研究对映体的常规动力学分辨具有重要意义。本研究还将重点了解分子包封和门控对碳氢化合物催化氧化的重要性。基于卟啉的篮子将被合成并用作模型来优化烯烃的氧化和烷烃中C-H键的激活，这些烷烃被选择性地封装在这些新宿主的腔内。Jovica Badjic教授将尝试了解C-H键的催化活化，这将使原料化学品有效地转化为有价值的产品。这项研究将为更有效地利用我们的碳基能源创造途径，从而造福社会。拟议的研究为具有挑战性的合成，有机光谱学，动力学，热力学和计算化学方面的学生和博士后提供了良好的培训，并将为这些学生未来在学术界或工业界的职业生涯做好准备。该计划旨在通过提高学生对我们社会在利用有限能源方面面临的挑战的认识，使研究和教学保持一致。该计划将帮助学生认识到超分子化学领域提供的研究机会，以创造更复杂的催化剂，其作用模式类似于酶。作为其多元化计划的一部分，该计划的重点是增加教师和研究生项目中未被充分代表的少数民族（URM）和女性的数量，PI将招收一名来自阿拉巴马农工大学（Alabama a&m University）的本科生，这是一所历史悠久的黑人大学。该学生将获得助学金，并在Badjic教授的研究小组度过一个夏天，以获得研究经验。

The Chemical Structure, Dynamics and Mechanisms Program supports Professor Jovica Badjic of Ohio State University for a project that will examine the utility of a new series of dynamic receptors - gated molecular baskets for developing concepts pertaining to an effective control of chemical reactivity in confined environments. Using computational and experimental tools, the researchers aim to understand and quantify the trafficking of multiple (more than one) molecules to and from molecular baskets, as well as to propose two new, self-assembling and folding, frameworks for controlling the dynamics of hosts and thereby the kinetics of molecular encapsulation. They also aim to gain kinetic control of the recognition by which chiral molecules enter/exit gated molecular hosts. The regulation of such kinetic discrimination via gating is important for developing methods for discriminating stereoisomeric compounds using artificial hosts and investigating a conventional kinetic resolution of enantiomers. This research will also focus on understanding the importance of molecular encapsulation and gating for catalytic oxidation of hydrocarbons. Porphyrin-based baskets will be synthesized and used as models to optimize the oxidation of alkenes and activation of C-H bonds in alkanes that are selectively encapsulated inside the cavity of these novel hosts.Professor Jovica Badjic will attempt to understand the catalytic activation of C-H bonds, which will allow the effective conversion of feedstock chemicals into valuable products. This study will benefit society by creating ways for more effective utilization of our carbon-based energy resources. The proposed research provides excellent training of students and postdocs in challenging syntheses, in organic spectroscopy, kinetics, thermodynamics and computational chemistry and will prepare these students for future careers in academia or industry. The proposed program is designed to align research and teaching by increasing students' awareness of the challenges that our society faces in utilizing limited energy resources. The program will help students to recognize research opportunities that the field of supramolecular chemistry offers toward creating more sophisticated catalysts with a mode of action resembling enzymes. As a part of their diversity plan that focuses on increasing the number of underrepresented minorities (URM) and women on the faculty and in their graduate program, the PI will host an undergraduate student from Alabama A&M University, an historically Black university. The student will be offered a stipend and spend a summer in Professor Badjic's research group to gain research experience.