An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding

Reaction of [U(TrenTIPS)] [1, TrenTIPS=N(CH2CH2NSiiPr3)3] with 0.25 equivalents of P4 reproducibly affords the unprecedented actinide inverted sandwich cyclo-P5 complex [{U(TrenTIPS)}2(μ-η5:η5-cyclo-P5)] (2). All prior examples of cyclo-P5 are stabilized by d-block metals, so 2 shows that cyclo-P5 d...

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Main Authors: Gardner, Benedict M., Tuna, Floriana, McInnes, Eric J.L., McMaster, Jonathan, Lewis, William, Blake, Alexander J., Liddle, Stephen T.
Format: Article
Published: Wiley-VCH Verlag 2015
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Online Access:https://eprints.nottingham.ac.uk/46638/
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author Gardner, Benedict M.
Tuna, Floriana
McInnes, Eric J.L.
McMaster, Jonathan
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
author_facet Gardner, Benedict M.
Tuna, Floriana
McInnes, Eric J.L.
McMaster, Jonathan
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
author_sort Gardner, Benedict M.
building Nottingham Research Data Repository
collection Online Access
description Reaction of [U(TrenTIPS)] [1, TrenTIPS=N(CH2CH2NSiiPr3)3] with 0.25 equivalents of P4 reproducibly affords the unprecedented actinide inverted sandwich cyclo-P5 complex [{U(TrenTIPS)}2(μ-η5:η5-cyclo-P5)] (2). All prior examples of cyclo-P5 are stabilized by d-block metals, so 2 shows that cyclo-P5 does not require d-block ions to be prepared. Although cyclo-P5 is isolobal to cyclopentadienyl, which usually bonds to metals via σ- and π-interactions with minimal δ-bonding, theoretical calculations suggest the principal bonding in the U(P5)U unit is polarized δ-bonding. Surprisingly, the characterization data are overall consistent with charge transfer from uranium to the cyclo-P5 unit to give a cyclo-P5 charge state that approximates to a dianionic formulation. This is ascribed to the larger size and superior acceptor character of cyclo-P5 compared to cyclopentadienyl, the strongly reducing nature of uranium(III), and the availability of uranium δ-symmetry 5f orbitals.
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spelling nottingham-466382020-05-04T17:07:21Z https://eprints.nottingham.ac.uk/46638/ An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding Gardner, Benedict M. Tuna, Floriana McInnes, Eric J.L. McMaster, Jonathan Lewis, William Blake, Alexander J. Liddle, Stephen T. Reaction of [U(TrenTIPS)] [1, TrenTIPS=N(CH2CH2NSiiPr3)3] with 0.25 equivalents of P4 reproducibly affords the unprecedented actinide inverted sandwich cyclo-P5 complex [{U(TrenTIPS)}2(μ-η5:η5-cyclo-P5)] (2). All prior examples of cyclo-P5 are stabilized by d-block metals, so 2 shows that cyclo-P5 does not require d-block ions to be prepared. Although cyclo-P5 is isolobal to cyclopentadienyl, which usually bonds to metals via σ- and π-interactions with minimal δ-bonding, theoretical calculations suggest the principal bonding in the U(P5)U unit is polarized δ-bonding. Surprisingly, the characterization data are overall consistent with charge transfer from uranium to the cyclo-P5 unit to give a cyclo-P5 charge state that approximates to a dianionic formulation. This is ascribed to the larger size and superior acceptor character of cyclo-P5 compared to cyclopentadienyl, the strongly reducing nature of uranium(III), and the availability of uranium δ-symmetry 5f orbitals. Wiley-VCH Verlag 2015-06-01 Article PeerReviewed Gardner, Benedict M., Tuna, Floriana, McInnes, Eric J.L., McMaster, Jonathan, Lewis, William, Blake, Alexander J. and Liddle, Stephen T. (2015) An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding. Angewandte Chemie International Edition, 54 (24). pp. 7068-7072. ISSN 1521-3773 cyclo-P5; density functional theory; phosphorus; uranium; δ bonding http://onlinelibrary.wiley.com/doi/10.1002/anie.201501728/abstract doi:10.1002/anie.201501728 doi:10.1002/anie.201501728
spellingShingle cyclo-P5; density functional theory; phosphorus; uranium; δ bonding
Gardner, Benedict M.
Tuna, Floriana
McInnes, Eric J.L.
McMaster, Jonathan
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title_full An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title_fullStr An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title_full_unstemmed An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title_short An inverted-sandwich diuranium μ-η5:η5-cyclo-P5 complex supported by U-P5 δ-bonding
title_sort inverted-sandwich diuranium μ-η5:η5-cyclo-p5 complex supported by u-p5 δ-bonding
topic cyclo-P5; density functional theory; phosphorus; uranium; δ bonding
url https://eprints.nottingham.ac.uk/46638/
https://eprints.nottingham.ac.uk/46638/
https://eprints.nottingham.ac.uk/46638/