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Synthesis of MOFs for Low Valent, Low Coordinate Metal Stabilization and Catalysis

Rabon, Allison Marie
http://rave.ohiolink.edu/etdc/view?acc_num=toledo1620508110773559

Abstract Details

2021, Doctor of Philosophy, University of Toledo, Chemistry.
Metal-organic frameworks (MOFs), a subset of coordination polymers, are a rapidly growing field. These 3D crystalline porous materials have the potential to enhance energy storage, catalysis, and toxic chemical remediation. MOF properties can be highly tuned, via pre or postsynthetic modification, to promote a seemingly infinite number of topologies that can be catered to one’s desired application. Our aim is to develop MOFs with post-synthetically introduced sensitive functionality to stabilize low valent and/or low coordinate metals for enhanced heterogeneous catalysis. Achieving this goal will minimize the use of nonrecoverable sterically bulky ligands that can be difficult/expensive to synthesize and replacing them with recyclable, low cost, robust networks. These frameworks will mimic the desirable features of homogeneous catalyst ligands allowing for stabilization of the low coordinate catalytic metal while allowing for comparable reactivity within a rigid heterogeneous material. Known frameworks, as well as PSM analogues with sensitive functionality, are currently being investigated for their stabilization of catalytic species for heterogeneous catalysis. Thermodynamically stable Zn 1D networks were synthesized using adb ligands instead of a desired porous 3D framework. We investigated concentration and solvent effects finding none that favor the desired 3D framework. A mixed ligand UiO-66 type framework, 90% UiO-66/UiO-66-NH2, was successfully synthesized and post-synthetically phosphorylated to obtain 90% UiO-66/UiO-66-NHPR2. This mixed ligand framework was tested for gold mediated cyclization of alkynes. MOF-808 was also successfully synthesized and post-synthetically phosphorylated to obtain MOF-808-2P and MOF-808-4P. These frameworks were tested for Suzuki-Miyaura cross-coupling, homocoupling of boronic acids, and gold mediated cyclization of alkynes. Finally, MOF-808 was investigated for the photothermal acetalization of aromatic aldehydes.
Michael Young, PhD (Advisor)
Mark Mason, PhD (Committee Member)
Joseph Schmidt, PhD (Committee Member)
Nikolas Podraza, PhD (Committee Member)
154 p.
Chemistry
Metal Organic Frameworks; MOFs; Catalysis; Acetalization;

Recommended Citations

Citations

  • Rabon, A. M. (2021). Synthesis of MOFs for Low Valent, Low Coordinate Metal Stabilization and Catalysis [Doctoral dissertation, University of Toledo]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=toledo1620508110773559

    APA Style (7th edition)

  • Rabon, Allison. Synthesis of MOFs for Low Valent, Low Coordinate Metal Stabilization and Catalysis. 2021. University of Toledo, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=toledo1620508110773559.

    MLA Style (8th edition)

  • Rabon, Allison. "Synthesis of MOFs for Low Valent, Low Coordinate Metal Stabilization and Catalysis." Doctoral dissertation, University of Toledo, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=toledo1620508110773559

    Chicago Manual of Style (17th edition)

toledo1620508110773559
163
© 2021, some rights reserved.Creative Commons License Synthesis of MOFs for Low Valent, Low Coordinate Metal Stabilization and Catalysis by Allison Marie Rabon is licensed under a Creative Commons Attribution-NonCommercial-NoDerivs 3.0 Unported License. Based on a work at etd.ohiolink.edu.
This open access ETD is published by University of Toledo and OhioLINK.