Uranium(III)-carbon multiple bonding supported by arene δ-bonding in mixed-valence hexauranium nanometre-scale rings
Abstract
Despite the fact that non-aqueous uranium chemistry is over 60 years old, most polarised-covalent uranium-element multiple bonds involve formal uranium oxidation states IV, V, and VI. The paucity of uranium(III) congeners is because, in common with metal-ligand multiple bonding generally, such linkages involve strongly donating, charge-loaded ligands that bind best to electron-poor metals and inherently promote disproportionation of uranium(III). Here, we report the synthesis of hexauranium-methanediide nanometre-scale rings. Combined experimental and computational studies suggest overall the presence of formal uranium(III) and (IV) ions, though electron delocalisation in this Kramers system cannot be definitively ruled out, and the resulting polarised-covalent U = C bonds are supported by iodide and δ-bonded arene bridges. The arenes provide reservoirs that accommodate charge, thus avoiding inter-electronic repulsion that would destabilise these low oxidation state metal-ligand multiple bonds. Using arenes as electronic buffers could constitute a general synthetic strategy by which to stabilise otherwise inherently unstable metal-ligand linkages.
- Authors:
-
[1];
[1];
[3];
[4];
[1]
- Univ. of Manchester (United Kingdom)
- Australian National Univ., Canberra, ACT (Australia)
- Univ. of Nottingham (United Kingdom)
- Univ. of Minnesota, Minneapolis, MN (United States)
- Publication Date:
- Research Org.:
- Univ. of Minnesota, Minneapolis, MN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1506462
- Grant/Contract Number:
- SC0002183
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Wooles, Ashley J., Mills, David P., Tuna, Floriana, McInnes, Eric J. L., Law, Gareth T. W., Fuller, Adam J., Kremer, Felipe, Ridgway, Mark, Lewis, William, Gagliardi, Laura, Vlaisavljevich, Bess, and Liddle, Stephen T. Uranium(III)-carbon multiple bonding supported by arene δ-bonding in mixed-valence hexauranium nanometre-scale rings. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-04560-7.
Wooles, Ashley J., Mills, David P., Tuna, Floriana, McInnes, Eric J. L., Law, Gareth T. W., Fuller, Adam J., Kremer, Felipe, Ridgway, Mark, Lewis, William, Gagliardi, Laura, Vlaisavljevich, Bess, & Liddle, Stephen T. Uranium(III)-carbon multiple bonding supported by arene δ-bonding in mixed-valence hexauranium nanometre-scale rings. United States. https://doi.org/10.1038/s41467-018-04560-7
Wooles, Ashley J., Mills, David P., Tuna, Floriana, McInnes, Eric J. L., Law, Gareth T. W., Fuller, Adam J., Kremer, Felipe, Ridgway, Mark, Lewis, William, Gagliardi, Laura, Vlaisavljevich, Bess, and Liddle, Stephen T. Tue .
"Uranium(III)-carbon multiple bonding supported by arene δ-bonding in mixed-valence hexauranium nanometre-scale rings". United States. https://doi.org/10.1038/s41467-018-04560-7. https://www.osti.gov/servlets/purl/1506462.
@article{osti_1506462,
title = {Uranium(III)-carbon multiple bonding supported by arene δ-bonding in mixed-valence hexauranium nanometre-scale rings},
author = {Wooles, Ashley J. and Mills, David P. and Tuna, Floriana and McInnes, Eric J. L. and Law, Gareth T. W. and Fuller, Adam J. and Kremer, Felipe and Ridgway, Mark and Lewis, William and Gagliardi, Laura and Vlaisavljevich, Bess and Liddle, Stephen T.},
abstractNote = {Despite the fact that non-aqueous uranium chemistry is over 60 years old, most polarised-covalent uranium-element multiple bonds involve formal uranium oxidation states IV, V, and VI. The paucity of uranium(III) congeners is because, in common with metal-ligand multiple bonding generally, such linkages involve strongly donating, charge-loaded ligands that bind best to electron-poor metals and inherently promote disproportionation of uranium(III). Here, we report the synthesis of hexauranium-methanediide nanometre-scale rings. Combined experimental and computational studies suggest overall the presence of formal uranium(III) and (IV) ions, though electron delocalisation in this Kramers system cannot be definitively ruled out, and the resulting polarised-covalent U = C bonds are supported by iodide and δ-bonded arene bridges. The arenes provide reservoirs that accommodate charge, thus avoiding inter-electronic repulsion that would destabilise these low oxidation state metal-ligand multiple bonds. Using arenes as electronic buffers could constitute a general synthetic strategy by which to stabilise otherwise inherently unstable metal-ligand linkages.},
doi = {10.1038/s41467-018-04560-7},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Tue May 29 00:00:00 EDT 2018},
month = {Tue May 29 00:00:00 EDT 2018}
}
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Fig. 1: Synthesis of complexes 2, 3, and 4 along with definitions of computational models used in this study. See ref. 43 for the synthesis of complex 2
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- Su, Wei; Pan, Sudip; Sun, Xiong
- Nature Communications, Vol. 9, Issue 1
DFT Investigations of the Magnetic Properties of Actinide Complexes
journal, February 2019
- Belkhiri, Lotfi; Le Guennic, Boris; Boucekkine, Abdou
- Magnetochemistry, Vol. 5, Issue 1
Mixed-valence Compounds: AuO 2 and AuS
journal, November 2018
- Tang, Meng; Zhang, Yanmei; Li, Siya
- ChemPhysChem, Vol. 19, Issue 22
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