Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex

The HAsAsH molecule has hitherto only been proposed tentatively as a short-lived species generated in electrochemical or microwave-plasma experiments. After two centuries of inconclusive or disproven claims of HAsAsH formation in the condensed phase, we report the isolation and structural authentica...

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Main Authors: Gardner, Benedict M., Balázs, Gábor, Scheer, Manfred, Wooles, Ashley J., Tuna, Floriana, McInnes, Eric J.L., McMaster, Jonathan, Lewis, William, Blake, Alexander J., Liddle, Stephen T.
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Published: Wiley-VCH Verlag 2015
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Online Access:https://eprints.nottingham.ac.uk/46637/
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author Gardner, Benedict M.
Balázs, Gábor
Scheer, Manfred
Wooles, Ashley J.
Tuna, Floriana
McInnes, Eric J.L.
McMaster, Jonathan
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
author_facet Gardner, Benedict M.
Balázs, Gábor
Scheer, Manfred
Wooles, Ashley J.
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 The HAsAsH molecule has hitherto only been proposed tentatively as a short-lived species generated in electrochemical or microwave-plasma experiments. After two centuries of inconclusive or disproven claims of HAsAsH formation in the condensed phase, we report the isolation and structural authentication of HAsAsH in the diuranium(IV) complex [{U(TrenTIPS)}2(μ-η2:η2-As2H2)] (3, TrenTIPS=N(CH2CH2NSiPri3)3; Pri=CH(CH3)2). Complex 3 was prepared by deprotonation and oxidative homocoupling of an arsenide precursor. Characterization and computational data are consistent with back-bonding-type interactions from uranium to the HAsAsH π*-orbital. This experimentally confirms the theoretically predicted excellent π-acceptor character of HAsAsH, and is tantamount to full reduction to the diarsane-1,2-diide form.
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spelling nottingham-466372020-05-04T17:27:52Z https://eprints.nottingham.ac.uk/46637/ Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex Gardner, Benedict M. Balázs, Gábor Scheer, Manfred Wooles, Ashley J. Tuna, Floriana McInnes, Eric J.L. McMaster, Jonathan Lewis, William Blake, Alexander J. Liddle, Stephen T. The HAsAsH molecule has hitherto only been proposed tentatively as a short-lived species generated in electrochemical or microwave-plasma experiments. After two centuries of inconclusive or disproven claims of HAsAsH formation in the condensed phase, we report the isolation and structural authentication of HAsAsH in the diuranium(IV) complex [{U(TrenTIPS)}2(μ-η2:η2-As2H2)] (3, TrenTIPS=N(CH2CH2NSiPri3)3; Pri=CH(CH3)2). Complex 3 was prepared by deprotonation and oxidative homocoupling of an arsenide precursor. Characterization and computational data are consistent with back-bonding-type interactions from uranium to the HAsAsH π*-orbital. This experimentally confirms the theoretically predicted excellent π-acceptor character of HAsAsH, and is tantamount to full reduction to the diarsane-1,2-diide form. Wiley-VCH Verlag 2015-12-07 Article PeerReviewed Gardner, Benedict M., Balázs, Gábor, Scheer, Manfred, Wooles, Ashley J., Tuna, Floriana, McInnes, Eric J.L., McMaster, Jonathan, Lewis, William, Blake, Alexander J. and Liddle, Stephen T. (2015) Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex. Angewandte Chemie International Edition, 54 (50). pp. 15250-15254. ISSN 1433-7851 arsenic; back-bonding; density functional theory; diarsene; uranium https://doi.org/10.1002/anie.201508600 10.1002/anie.201508600 10.1002/anie.201508600 10.1002/anie.201508600
spellingShingle arsenic; back-bonding; density functional theory; diarsene; uranium
Gardner, Benedict M.
Balázs, Gábor
Scheer, Manfred
Wooles, Ashley J.
Tuna, Floriana
McInnes, Eric J.L.
McMaster, Jonathan
Lewis, William
Blake, Alexander J.
Liddle, Stephen T.
Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title_full Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title_fullStr Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title_full_unstemmed Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title_short Isolation of elusive HAsAsH in a crystalline diuranium(IV) complex
title_sort isolation of elusive hasash in a crystalline diuranium(iv) complex
topic arsenic; back-bonding; density functional theory; diarsene; uranium
url https://eprints.nottingham.ac.uk/46637/
https://eprints.nottingham.ac.uk/46637/
https://eprints.nottingham.ac.uk/46637/