Synthesis of a diruthenium μ-η<sup>4</sup>-α-diimine complex <i>via</i> dehydrogenative coupling of cyclic amines and its role in dehydrogenative oxidation of pyrrolidine

Takao, Toshiro; Shimogawa, Ryuichi; Fujita, Ryosuke; Egawa, Shu

doi:10.1039/d3dt03187j

Dalton Trans.

2023

DOI: 10.1039/d3dt03187j

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Synthesis of a diruthenium μ-η⁴-α-diimine complex via dehydrogenative coupling of cyclic amines and its role in dehydrogenative oxidation of pyrrolidine

Toshiro Takao,

Ryuichi Shimogawa,

Ryosuke Fujita

et al.

Abstract: The reaction of [Cp‡Ru(μ-H)4RuCp‡] (1: Cp‡ = 1,2,4-tri-tert-butylcyclopentadienyl) with cyclic amines at 180 °C afforded μ-η4-α-diimine complex, [(Cp‡Ru)2(μ-η4-C2nH4n–4N2)] (5a-c: n = 4, 5, 6) via dehydrogenative coupling of two cyclic...

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2024

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Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

Takao,

Matsuzawa,

Nagaoka

2024

Inorg. Chem.

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Heterometallic tetrahydrido complexes [Cp*Re(H) 2 (μ-H) 2 MCp*] (5a: M = Ir, 5b: M = Rh) were synthesized by the reaction of [Cp*ReH 6 ] and [Cp*M(sol) 3 ] 2+ (M = Ir, Rh) followed by deprotonation. Although 5 possesses four hydrides and adopts a 30electron configuration as [Cp*Ru(μ-H) 4 RuCp*] (1) does, the positions of the hydrides in 5 differ from those in 1: two terminal and two bridging hydrides. In addition, adaptive natural density partitioning (AdNDP) analysis demonstrated that a direct Re−M bond is held in 5. Although cationic pentahydrido complexes [Cp*Re(H) 2 (μ-H) 3 MCp*] + (4a: M = Ir, 4b: M = Rh) do not contain a direct Re−M bond, the formation of a Re−M bond in the intermediate of the hydride site exchange was also inferred by DFT calculations. DFT calculations suggested that the Re−M bond plays a crucial role in the site exchange of hydrides in 5 and 4. While μ-phosphido complex [Cp*(PPh 3 )Re(H)(μ-H)(μ-PPh 2 )Ir(H)Cp*] (6) was obtained by the reaction of 5a with PPh 3 , the treatment of 5a with PMe 3 resulted in the formation of a 1:1 mixture of [Cp*Re(H) 2 (PMe 3 ) 2 ] and [Cp*Ir(H) 2 PMe 3 ] via the rupture of the Re−Ir bond.

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Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

Takao,

Matsuzawa,

Nagaoka

2024

Inorg. Chem.

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Synthesis of a diruthenium μ-η⁴-α-diimine complex via dehydrogenative coupling of cyclic amines and its role in dehydrogenative oxidation of pyrrolidine

Abstract: The reaction of [Cp‡Ru(μ-H)4RuCp‡] (1: Cp‡ = 1,2,4-tri-tert-butylcyclopentadienyl) with cyclic amines at 180 °C afforded μ-η4-α-diimine complex, [(Cp‡Ru)2(μ-η4-C2nH4n–4N2)] (5a-c: n = 4, 5, 6) via dehydrogenative coupling of two cyclic...

Cited by 1 publication

References 78 publications

Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

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Synthesis of a diruthenium μ-η4-α-diimine complex via dehydrogenative coupling of cyclic amines and its role in dehydrogenative oxidation of pyrrolidine

Abstract: The reaction of [Cp‡Ru(μ-H)4RuCp‡] (1: Cp‡ = 1,2,4-tri-tert-butylcyclopentadienyl) with cyclic amines at 180 °C afforded μ-η4-α-diimine complex, [(Cp‡Ru)2(μ-η4-C2nH4n–4N2)] (5a-c: n = 4, 5, 6) via dehydrogenative coupling of two cyclic...

Cited by 1 publication

References 78 publications

Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

Synthesis of Bimetallic Dinuclear Hydrido Complexes of Re and Rh/Ir Supported by a Direct M–M′ Bond: The Role of the M–M′ Bond in the Site Exchange of Hydrides

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Synthesis of a diruthenium μ-η⁴-α-diimine complex via dehydrogenative coupling of cyclic amines and its role in dehydrogenative oxidation of pyrrolidine