Non-Technical Abstract:<br/>Metal-organic frameworks (MOFs) are materials that continue to gain interest from the materials research community for their potential in industrial applications such as catalysis, purification, and molecular storage. The scalability of MOF syntheses has always been a barrier to large scale industrial implementation, in which some frameworks either do not form at all or have diminished materials properties upon scaling. While the community has developed several methods for the synthesis of these materials, the fundamental chemistry behind their formation remains to be elucidated. This project focuses on understanding the mechanism of MOF formation at the early stages of their assembly, leading to advances in rational design, scalable synthesis, and increased industrial relevance. Through synergistically combining the synthesis of new materials and utilizing spectroscopy a detailed understanding of MOF formation is being developed. Such approaches have been the hallmark of other synthetic fields including the pharmaceutical industry in which a rich understanding of mechanistic organic chemistry has directly led to the synthesis of blockbuster drugs. To increase adult scientific literacy, a lecture series at the Mahoning Valley Lifelong Learning Institute (MVLLI), an adult-centered education facility, focusing on demystifying materials chemistry has been initiated. <br/><br/>Technical Abstract:<br/>The research activities focus on understanding the mechanism of formation of the inorganic secondary building units (SBUs) in metal-organic framework (MOF) architectures. This project outlines a spectroscopic and synthetic road map to gain mechanistic understanding of the formation of the SBU and the subsequent self-assembly process. This level of understanding is expected to lead to more efficient syntheses of MOFs and to novel framework architectures with untold properties that were previously inaccessible. Raman spectroscopy is used to identify solution-phase intermediates prior to the precipitation of the fully formed MOF (Objective 1). The identified intermediates are then targeted for independent synthesis in either molecular or polymeric form (Objective 2). The synthesized intermediates are subjected to further chemistry which yields electronically diverse copolymers that cannot be realized by traditional means (Objective 3). Undergraduate and Master level students are involved in all aspects of this project from MOF syntheses and spectroscopy to delivering lectures for the adult outreach program.<br/><br/>This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.