Evidence of a Uranium‐Paddlewheel Node in a Catecholate‐Based Metal–Organic Framework

Knapp, Julia G.; Wang, Xijun; Rosen, Andrew S.; Wang, Xingjie; Gong, Xinyi; Schneider, Matthew; Elkin, Tatyana; Kirlikovali, Kent O.; Fairley, Melissa; Krzyaniak, Matthew D.; Wasielewski, Michael R.; Gianneschi, Nathan C.; Snurr, Randall Q.; Farha, Omar K.

doi:10.1002/ange.202305526

Evidence of a Uranium‐Paddlewheel Node in a Catecholate‐Based Metal–Organic Framework

Journal Article · Mon Jun 12 00:00:00 EDT 2023 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202305526· OSTI ID:1984717

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Department of Chemistry Northwestern University 2145 Sheridan Rd. Evanston IL 60208 USA
Department of Chemical and Biological Engineering Northwestern University 2145 Sheridan Rd. Evanston IL 60208 USA
Department of Materials Science and Engineering University of California, Berkeley 2607 Hearst Ave Berkeley CA 94720 USA
Los Alamos National Laboratory Los Alamos NM 87544 USA
Notre Dame Radiation Laboratory University of Notre Dame Notre Dame IN 46556 USA

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 U ⁴⁺ ‐paddlewheel nodes and catecholate‐based linkers. We propose this highly unusual structure, which contains two U ⁴⁺ 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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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; FG02-03ER15457; NA0003763

OSTI ID:: 1984717

Alternate ID(s):: OSTI ID: 1989247

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 29 Vol. 135; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Evidence of a Uranium‐Paddlewheel Node in a Catecholate‐Based Metal–Organic Framework

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