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

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

doi:10.1002/anie.202305526

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

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

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

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.

Original language	English (US)
Article number	e202305526
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	29
DOIs	https://doi.org/10.1002/anie.202305526
State	Published - Jul 17 2023
Externally published	Yes

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry

Keywords

Catecholate
Metal–Organic Framework
Uranium

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10.1002/anie.202305526

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Knapp, J. G., Wang, X., Rosen, A. S., Wang, X., Gong, X., Schneider, M., Elkin, T., Kirlikovali, K. O., Fairley, M., Krzyaniak, M. D., Wasielewski, M. R., Gianneschi, N. C., Snurr, R. Q., & Farha, O. K. (2023). Evidence of a Uranium-Paddlewheel Node in a Catecholate-Based Metal–Organic Framework. Angewandte Chemie - International Edition, 62(29), Article e202305526. https://doi.org/10.1002/anie.202305526

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title = "Evidence of a Uranium-Paddlewheel Node in a Catecholate-Based Metal–Organic Framework",

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.",

keywords = "Catecholate, Metal–Organic Framework, Uranium",

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

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doi = "10.1002/anie.202305526",

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Knapp, JG, Wang, X, Rosen, AS, Wang, X, Gong, X, Schneider, M, Elkin, T, Kirlikovali, KO, Fairley, M, Krzyaniak, MD, Wasielewski, MR, Gianneschi, NC, Snurr, RQ & Farha, OK 2023, 'Evidence of a Uranium-Paddlewheel Node in a Catecholate-Based Metal–Organic Framework', Angewandte Chemie - International Edition, vol. 62, no. 29, e202305526. https://doi.org/10.1002/anie.202305526

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T1 - Evidence of a Uranium-Paddlewheel Node in a Catecholate-Based Metal–Organic Framework

AU - Knapp, Julia G.

AU - Wang, Xijun

AU - Rosen, Andrew S.

AU - Wang, Xingjie

AU - Gong, Xinyi

AU - Schneider, Matthew

AU - Elkin, Tatyana

AU - Kirlikovali, Kent O.

AU - Fairley, Melissa

AU - Krzyaniak, Matthew D.

AU - Wasielewski, Michael R.

AU - Gianneschi, Nathan C.

AU - Snurr, Randall Q.

AU - Farha, Omar K.

PY - 2023/7/17

Y1 - 2023/7/17

N2 - 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.

AB - 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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KW - Metal–Organic Framework

KW - Uranium

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

Abstract

All Science Journal Classification (ASJC) codes

Keywords

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