Activation of CO by hydrogenated magnesium(I) dimers: sterically controlled formation of ethenediolate and cyclopropanetriolate complexes

Ralte Lalrempuia, Christos E Kefalidis, Simon James Bonyhady, Benedikt Schwarze, Laurent Maron, Andreas Stasch, Cameron Jones

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Abstract

This study details the formal hydrogenation of two magnesium(I) dimers {(Nacnac)Mg}2 (Nacnac = [{(C6H3R2-2,6)NCMe}2CH]−; R = Pri (DipNacnac), Et (DepNacnac)) using 1,3-cyclohexadiene. These reactions afford the magnesium(II) hydride complexes, {(Nacnac)Mg(μ-H)}2. Their reactions with excess CO are sterically controlled and lead cleanly to different C–C coupled products, viz. the ethenediolate complex, (DipNacnac)Mg{κ1-O-[(DipNacnac)Mg(κ2-O,O-O2C2H2)]}, and the first cyclopropanetriolate complex of any metal, cis-{(DepNacnac)Mg}3{μ-C3(H3)O3}. Computational studies imply the CO activation processes proceed via very similar mechanisms to those previously reported for related reactions involving f-block metal hydride compounds. This work highlights the potential magnesium compounds hold for use in the “Fischer–Tropsch-like” transformation of CO/H2 mixtures to value added oxygenate products.
Original languageEnglish
Pages (from-to)8944-8947
Number of pages4
JournalJournal of the American Chemical Society
Volume137
Issue number28
DOIs
Publication statusPublished - 2015

Cite this

Lalrempuia, Ralte ; Kefalidis, Christos E ; Bonyhady, Simon James ; Schwarze, Benedikt ; Maron, Laurent ; Stasch, Andreas ; Jones, Cameron. / Activation of CO by hydrogenated magnesium(I) dimers: sterically controlled formation of ethenediolate and cyclopropanetriolate complexes. In: Journal of the American Chemical Society. 2015 ; Vol. 137, No. 28. pp. 8944-8947.
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title = "Activation of CO by hydrogenated magnesium(I) dimers: sterically controlled formation of ethenediolate and cyclopropanetriolate complexes",
abstract = "This study details the formal hydrogenation of two magnesium(I) dimers {(Nacnac)Mg}2 (Nacnac = [{(C6H3R2-2,6)NCMe}2CH]−; R = Pri (DipNacnac), Et (DepNacnac)) using 1,3-cyclohexadiene. These reactions afford the magnesium(II) hydride complexes, {(Nacnac)Mg(μ-H)}2. Their reactions with excess CO are sterically controlled and lead cleanly to different C–C coupled products, viz. the ethenediolate complex, (DipNacnac)Mg{κ1-O-[(DipNacnac)Mg(κ2-O,O-O2C2H2)]}, and the first cyclopropanetriolate complex of any metal, cis-{(DepNacnac)Mg}3{μ-C3(H3)O3}. Computational studies imply the CO activation processes proceed via very similar mechanisms to those previously reported for related reactions involving f-block metal hydride compounds. This work highlights the potential magnesium compounds hold for use in the “Fischer–Tropsch-like” transformation of CO/H2 mixtures to value added oxygenate products.",
author = "Ralte Lalrempuia and Kefalidis, {Christos E} and Bonyhady, {Simon James} and Benedikt Schwarze and Laurent Maron and Andreas Stasch and Cameron Jones",
year = "2015",
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Activation of CO by hydrogenated magnesium(I) dimers: sterically controlled formation of ethenediolate and cyclopropanetriolate complexes. / Lalrempuia, Ralte; Kefalidis, Christos E; Bonyhady, Simon James; Schwarze, Benedikt; Maron, Laurent; Stasch, Andreas; Jones, Cameron.

In: Journal of the American Chemical Society, Vol. 137, No. 28, 2015, p. 8944-8947.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - Activation of CO by hydrogenated magnesium(I) dimers: sterically controlled formation of ethenediolate and cyclopropanetriolate complexes

AU - Lalrempuia, Ralte

AU - Kefalidis, Christos E

AU - Bonyhady, Simon James

AU - Schwarze, Benedikt

AU - Maron, Laurent

AU - Stasch, Andreas

AU - Jones, Cameron

PY - 2015

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N2 - This study details the formal hydrogenation of two magnesium(I) dimers {(Nacnac)Mg}2 (Nacnac = [{(C6H3R2-2,6)NCMe}2CH]−; R = Pri (DipNacnac), Et (DepNacnac)) using 1,3-cyclohexadiene. These reactions afford the magnesium(II) hydride complexes, {(Nacnac)Mg(μ-H)}2. Their reactions with excess CO are sterically controlled and lead cleanly to different C–C coupled products, viz. the ethenediolate complex, (DipNacnac)Mg{κ1-O-[(DipNacnac)Mg(κ2-O,O-O2C2H2)]}, and the first cyclopropanetriolate complex of any metal, cis-{(DepNacnac)Mg}3{μ-C3(H3)O3}. Computational studies imply the CO activation processes proceed via very similar mechanisms to those previously reported for related reactions involving f-block metal hydride compounds. This work highlights the potential magnesium compounds hold for use in the “Fischer–Tropsch-like” transformation of CO/H2 mixtures to value added oxygenate products.

AB - This study details the formal hydrogenation of two magnesium(I) dimers {(Nacnac)Mg}2 (Nacnac = [{(C6H3R2-2,6)NCMe}2CH]−; R = Pri (DipNacnac), Et (DepNacnac)) using 1,3-cyclohexadiene. These reactions afford the magnesium(II) hydride complexes, {(Nacnac)Mg(μ-H)}2. Their reactions with excess CO are sterically controlled and lead cleanly to different C–C coupled products, viz. the ethenediolate complex, (DipNacnac)Mg{κ1-O-[(DipNacnac)Mg(κ2-O,O-O2C2H2)]}, and the first cyclopropanetriolate complex of any metal, cis-{(DepNacnac)Mg}3{μ-C3(H3)O3}. Computational studies imply the CO activation processes proceed via very similar mechanisms to those previously reported for related reactions involving f-block metal hydride compounds. This work highlights the potential magnesium compounds hold for use in the “Fischer–Tropsch-like” transformation of CO/H2 mixtures to value added oxygenate products.

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