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Electronic Communication in Binuclear Osmium- and Iridium-Polyhydrides.

ABSTRACT: Reactions of polyhydrides OsH₆(PⁱPr₃)₂ (1) and IrH₅(PⁱPr₃)₂ (2) with rollover cyclometalated hydride complexes have been investigated in order to explore the influence of a metal center on the MH_n unit of the other in mixed valence binuclear polyhydrides. Hexahydride 1 activates an ortho-CH bond of the heterocyclic moiety of the trihydride metal-ligand compounds OsH₃{κ²-C,N-[C₅RH₂N-py]}(PⁱPr₃)₂ (R = H (3), Me (4), Ph (5)). Reactions of 3 and 4 lead to the hexahydrides (PⁱPr₃)₂H₃Os{μ-[κ²-C,N-[C₅RH₂N-C₅H₃N]-N,C-κ²]}OsH₃(PⁱPr₃)₂ (R = H (6), Me (7)), whereas 5 gives the pentahydride (PⁱPr₃)₂H₃Os{μ-[κ²-C,N-[C₅H₃N-C₅(C₆H₄)H₂N]-C,N,C-κ³]}OsH₂(PⁱPr₃)₂ (8). Pentahydride 2 promotes C-H bond activation of 3 and the iridium-dihydride IrH₂{κ²-C,N-[C₅H₃N-py]}(PⁱPr₃)₂ (9) to afford the heterobinuclear pentahydride (PⁱPr₃)₂H₃Os{μ-[κ²-C,N-[C₅H₃N-C₅H₃N]-N,C-κ²]}IrH₂(PⁱPr₃)₂ (10) and the homobinuclear tetrahydride (PⁱPr₃)₂H₂Ir{μ-[κ²-C,N-[C₅H₃N-C₅H₃N]-N,C-κ²]}IrH₂(PⁱPr₃)₂ (11), respectively. Complexes 6-8 and 11 display HOMO delocalization throughout the metal-heterocycle-metal skeleton. Their sequential oxidation generates mono- and diradicals, which exhibit intervalence charge transfer transitions. This notable ability allows the tuning of the strength of the hydrogen-hydrogen and metal-hydrogen interactions within the MH_n units.

SUBMITTER: Cancela L

PROVIDER: S-EPMC9179948 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Electronic Communication in Binuclear Osmium- and Iridium-Polyhydrides.

Cancela Lara L Esteruelas Miguel A MA Galbán Javier J Oliván Montserrat M Oñate Enrique E Vélez Andrea A Vidal Juan C JC

Inorganic chemistry 20210205 4

Reactions of polyhydrides OsH6(PiPr3)2 (1) and IrH5(PiPr3)2 (2) with rollover cyclometalated hydride complexes have been investigated in order to explore the influence of a metal center on the MHn unit of the other in mixed valence binuclear polyhydrides. Hexahydride 1 activates an ortho-CH bond of the heterocyclic moiety of the trihydride metal-ligand compounds O ...[more]

PMID: 33543934

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Electronic Communication in Binuclear Osmium- and Iridium-Polyhydrides.

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Electronic Communication in Binuclear Osmium- and Iridium-Polyhydrides.

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