Evidence of a Uranium-Paddlewheel Node in a Catecholate-Based Metal–Organic Framework |
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| Authors: | Julia G Knapp Dr Xijun Wang Dr Andrew S Rosen Xingjie Wang Dr Xinyi Gong Dr Matthew Schneider Dr Tatyana Elkin Dr Kent O Kirlikovali Dr Melissa Fairley Dr Matthew D Krzyaniak Prof Michael R Wasielewski Prof Nathan C Gianneschi Prof Randall Q Snurr Prof Omar K Farha |
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| Institution: | 1. Department of Chemistry, Northwestern University, 2145 Sheridan Rd., Evanston, IL 60208 USA;2. Department of Chemical and Biological Engineering, Northwestern University, 2145 Sheridan Rd., Evanston, IL 60208 USA;3. Department of Materials Science and Engineering, University of California, Berkeley, 2607 Hearst Ave, Berkeley, CA 94720 USA;4. Los Alamos National Laboratory, Los Alamos, NM 87544 USA;5. Notre Dame Radiation Laboratory, University of Notre Dame, Notre Dame, IN 46556 USA |
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| Abstract: | The interactions between uranium and non-innocent organic species are an essential component of fundamental uranium redox chemistry. However, they have seldom been explored in the context of multidimensional, porous materials. Uranium-based metal–organic frameworks (MOFs) offer a new angle to study these interactions, as these self-assembled species stabilize uranium species through immobilization by organic linkers within a crystalline framework, while potentially providing a method for adjusting metal oxidation state through coordination of non-innocent linkers. We report the synthesis of the MOF NU-1700 , assembled from U4+-paddlewheel nodes and catecholate-based linkers. We propose this highly unusual structure, which contains two U4+ ions in a paddlewheel built from four linkers—a first among uranium materials—as a result of extensive characterization via powder X-ray diffraction (PXRD), sorption, transmission electron microscopy (TEM), and thermogravimetric analysis (TGA), in addition to density functional theory (DFT) calculations. |
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| Keywords: | Catecholate Metal–Organic Framework Uranium |
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