Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride

Deprotonation of [U(TrenTIPS)(NH2)] (1) [TrenTIPS = N(CH2CH2NSiPri3)3] with organoalkali metal reagents MR (M = Li, R = But; M = Na−Cs, R = CH2C6H5) afforded the imido-bridged dimers [{U-(TrenTIPS)(μ-N[H]M)}2] [M = L −Cs (2a−e)]. Treatmentof 2c (M = K) with 2 equiv of 15 crown-5 ether (15C5) afforde...

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Main Authors: King, David M., McMaster, Jonathan, Tuna, Floriana, McInnes, Eric J.L., Lewis, William, Blake, Alexander J., Liddle, Stephen T.
Format: Article
Published: American Chemical Society 2014
Online Access:https://eprints.nottingham.ac.uk/35876/
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author King, David M.
McMaster, Jonathan
Tuna, Floriana
McInnes, Eric J.L.
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
author_facet King, David M.
McMaster, Jonathan
Tuna, Floriana
McInnes, Eric J.L.
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
author_sort King, David M.
building Nottingham Research Data Repository
collection Online Access
description Deprotonation of [U(TrenTIPS)(NH2)] (1) [TrenTIPS = N(CH2CH2NSiPri3)3] with organoalkali metal reagents MR (M = Li, R = But; M = Na−Cs, R = CH2C6H5) afforded the imido-bridged dimers [{U-(TrenTIPS)(μ-N[H]M)}2] [M = L −Cs (2a−e)]. Treatmentof 2c (M = K) with 2 equiv of 15 crown-5 ether (15C5) afforded the uranium terminal parent imido complex [U(TrenTIPS)(NH)][K(15C5)2] (3c), which can also be viewed as a masked uranium(IV) nitride. The uranium−imido linkage was found to be essentially linear, and theoretical calculations suggested σ2π4 polarized U−N multiple bonding. Attempts to oxidize 3c to afford the neutral uranium terminal parent imido complex [U(TrenTIPS)(NH)] (4) resulted in spontaneous disproportionation to give 1 and the uranium−nitride complex [U(TrenTIPS)(N)] (5); this reaction is a new way to prepare the terminal uranium−nitride linkage and was calculated to be exothermic by −3.25 kcal mol−1.
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spelling nottingham-358762020-05-04T16:47:09Z https://eprints.nottingham.ac.uk/35876/ Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride King, David M. McMaster, Jonathan Tuna, Floriana McInnes, Eric J.L. Lewis, William Blake, Alexander J. Liddle, Stephen T. Deprotonation of [U(TrenTIPS)(NH2)] (1) [TrenTIPS = N(CH2CH2NSiPri3)3] with organoalkali metal reagents MR (M = Li, R = But; M = Na−Cs, R = CH2C6H5) afforded the imido-bridged dimers [{U-(TrenTIPS)(μ-N[H]M)}2] [M = L −Cs (2a−e)]. Treatmentof 2c (M = K) with 2 equiv of 15 crown-5 ether (15C5) afforded the uranium terminal parent imido complex [U(TrenTIPS)(NH)][K(15C5)2] (3c), which can also be viewed as a masked uranium(IV) nitride. The uranium−imido linkage was found to be essentially linear, and theoretical calculations suggested σ2π4 polarized U−N multiple bonding. Attempts to oxidize 3c to afford the neutral uranium terminal parent imido complex [U(TrenTIPS)(NH)] (4) resulted in spontaneous disproportionation to give 1 and the uranium−nitride complex [U(TrenTIPS)(N)] (5); this reaction is a new way to prepare the terminal uranium−nitride linkage and was calculated to be exothermic by −3.25 kcal mol−1. American Chemical Society 2014-04-03 Article PeerReviewed King, David M., McMaster, Jonathan, Tuna, Floriana, McInnes, Eric J.L., Lewis, William, Blake, Alexander J. and Liddle, Stephen T. (2014) Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride. Journal of the American Chemical Society, 136 (15). pp. 5619-5622. ISSN 1520-5126 http://pubs.acs.org/doi/abs/10.1021/ja502405e doi:10.1021/ja502405e doi:10.1021/ja502405e
spellingShingle King, David M.
McMaster, Jonathan
Tuna, Floriana
McInnes, Eric J.L.
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title_full Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title_fullStr Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title_full_unstemmed Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title_short Synthesis and characterization of an f‑block terminal parent imido [U=NH] complex: a masked uranium(IV) nitride
title_sort synthesis and characterization of an f‑block terminal parent imido [u=nh] complex: a masked uranium(iv) nitride
url https://eprints.nottingham.ac.uk/35876/
https://eprints.nottingham.ac.uk/35876/
https://eprints.nottingham.ac.uk/35876/