N N bond cleavage upon reduction and protonation of phenylazophenylate coordinated to ruthenium complex

Tomioka, Nozomi; Misawa‐Suzuki, Tomoyo; Nagao, Hidemi

doi:10.1016/j.poly.2021.115193

Cited by 6 publications

(1 citation statement)

References 57 publications

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“…It was revealed that the {Ru 2 III,IV (μ-O) 2 (μ-O 2 CO)} + core was stable in all the pH regions and two-step protonation/ deprotonation reversibly occurred, although there has been reports on the decarboxylation of CO 3 2− under strongly acidic conditions on the metal centers. 11,14 Interactions with M + even in solutions would contribute to preventing decarboxylation in our system.…”

Section: ■ Results and Discussionmentioning

confidence: 97%

Synthesis of Carbonato- and Doubly Oxido-Bridged Diruthenium(III,IV) Complex and Reactions with Cations

2021

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Doubly oxido-bridged transition metal moieties, {M 2 (μ-O) 2 }, play important roles as oxidation reaction centers in nature. This work features a diruthenium(III,IV) complex with a doubly oxido-bridged core {Ru 2 III,IV (μ-O) 2 } 3+ with a carbonato bridged between the two ruthenium centers, M[{Ru III,IV (ebpma)} 2 (μ-O) 2 (μ-O 2 CO)] 2 (PF 6 ) 3 (M[1 CO3 ] 2 (PF 6 ) 3 ; Carbonato complex, ebpma; ethylbis(2-pyridymethyl)amine), and explores the interactions of this complex with cations (H + and M + ). M[1 CO3 ] 2 (PF 6 ) 3 was formed via reactions of a singly oxido-bridged complex, [{Ru III,IV Cl 2 (ebpma)} 2 (μ-O)]PF 6 •(CH 3 ) 2 CO, with M 2 CO 3 (M = K, Na) or with CO 2 (g), adjusted to around pH 12 with NaOH(aq.), in a water−acetone mixed solvent. The Carbonato complex was isolated as a powder in the form of M[1 CO3 ] 2 (PF 6 ) 3 (M = K, Na), because of the interactions between the carbonato moiety and K + or Na + in the solid structure. In acidic aqueous solutions, unexpectedly, the carbonato ligand remained bound to the doubly bridged core, {Ru 2 III,IV (μ-O) 2 } 3+ or {Ru 2 III,IV (μ-O)(μ−OH)} 4+ , without decarboxylation even under pH 1.0. Two-step one-protonation/ deprotonation occurred reversibly between pH 1.0 and 13.2 to the bridging oxido and carbonato ligands. The structures of the corresponding one-and two-protonated complexes ([1 CO3 H] 2+ and [1 CO3 2H] 3+ ) were successfully characterized.

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Section: ■ Results and Discussionmentioning

confidence: 97%

Synthesis of Carbonato- and Doubly Oxido-Bridged Diruthenium(III,IV) Complex and Reactions with Cations

2021

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A Conjugated Covalent Template Strategy for All‐Benzene Catenane Synthesis

Zhao

Xiao

et al. 2022

Angewandte Chemie

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Mechanically interlocked molecules based on oligoparaphenylene‐derived nanohoops, particularly those without heteroatoms, are synthetically challenging and topologically intriguing targets. Herein, a π‐conjugated covalent template strategy based on azo group has been developed, which features dual intramolecular macrocyclizations directed by a tetra‐substituted azobenzene core, followed by traceless removal of the azo linker. Employing this strategy, the efficient synthesis of a novel all‐benzene [2]catenane consisting of meta‐cycloparaphenylenes has been accomplished.

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A Conjugated Covalent Template Strategy for All‐Benzene Catenane Synthesis

Zhao

Xiao

et al. 2022

Angew Chem Int Ed

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Mechanically interlocked molecules based on oligoparaphenylene-derived nanohoops, particularly those without heteroatoms, are synthetically challenging and topologically intriguing targets. Herein, a π-conjugated covalent template strategy based on azo group has been developed, which features dual intramolecular macrocyclizations directed by a tetra-substituted azobenzene core, followed by traceless removal of the azo linker. Employing this strategy, the efficient synthesis of a novel all-benzene [2]catenane consisting of meta-cycloparaphenylenes has been accomplished.

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N N bond cleavage upon reduction and protonation of phenylazophenylate coordinated to ruthenium complex

Cited by 6 publications

References 57 publications

Synthesis of Carbonato- and Doubly Oxido-Bridged Diruthenium(III,IV) Complex and Reactions with Cations

Synthesis of Carbonato- and Doubly Oxido-Bridged Diruthenium(III,IV) Complex and Reactions with Cations

A Conjugated Covalent Template Strategy for All‐Benzene Catenane Synthesis

A Conjugated Covalent Template Strategy for All‐Benzene Catenane Synthesis

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