A pyrazine‐bridged trimer of oxo‐centered triruthenium–carbonyl clusters and the supramolecular assembly built from multiple noncovalent contacts

Daicho, Keita; Ozawa, Yoshiki; Sugimoto, Kunihisa; Abe, Masaaki

doi:10.1002/jccs.202000491

Cited by 3 publications

(1 citation statement)

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“…We use the layer-by-layer method to obtain polyruthenated porphyrin films organized in stacked structures − and the LB technology to obtain films of amphiphilic − and non-amphiphilic ruthenium complexes and heterostructured films combining highly ordered structures and electroactive ruthenium complexes . We note that the electrochemical response of multilayer films fabricated with the LB method was influenced by the molecule geometry and molecular packing. , Likewise, it was demonstrated that designing the interactions and components within the multilayer structures with ruthenium complexes could lead to highly organized structures with tuned properties, − such as fast electronic transport within the film. , The tailored films are especially suitable for electrochemical energy conversion and storage devices since their functioning relies on processes occurring at the electrode–electrolyte interface (e.g., electron transfer across the interface). − …”

Section: Introductionmentioning

confidence: 99%

Understanding the Electrochemistry of Ruthenium Complex Thin Films to Guide the Design of Improved Energy Storage Electrodes

Mendoza

Winnischofer

2021

J. Phys. Chem. C

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Materials with fast charge transfer processes across electrochemical interfaces could exhibit a pseudocapacitive behavior, which is promising to achieve both high power and high energy density in energy storage devices. Therefore, the design of electrodes with highly exposed electroactive species and improved charge transport should lead to pseudocapacitive electrodes with high capacity at high rates. Herein, redox thin-film electrodes based on amphiphilic tri-ruthenium clusters are constructed and evaluated as energy storage electrodes. Cyclic voltammetry results are interpreted with the aid of a mathematical model, which describes the electrochemical response of layered films considering the stability of molecules and the charge transfer within the film. It is found that the interactions between tri-ruthenium cluster molecules within the film and the relatively fast electron transfer at the substrate/film interface lead to a wide redox peak with capacitive characteristics, achieving a specific capacitance of 204 F g–1 (1.02 mF cm2) for the electrode with 18 monolayers. However, the efficiency at high rates of thicker electrodes should be improved, and the model suggests that electron transfer at the substrate/film interface and the charge transport within the film are key factors to improving the energy storage efficiency at high rates in film electrodes.

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Section: Introductionmentioning

confidence: 99%

Understanding the Electrochemistry of Ruthenium Complex Thin Films to Guide the Design of Improved Energy Storage Electrodes

Mendoza

Winnischofer

2021

J. Phys. Chem. C

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Oxo-centered trinuclear ruthenium acetates: Structure and applications

Nikolaou¹,

Nascimento²,

Alexiou³

2023

Coordination Chemistry Reviews

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Synthetic, Electrochemical, DFT, and Synchrotron X-ray Charge-Density Studies on Oxo-centered Triruthenium Clusters Supported by Electron-Withdrawing Carboxylates

Tahara,

Morino,

Morimoto

et al. 2024

Inorg. Chem.

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We herein report the synthesis, characterizations, and synchrotron X-ray charge-density studies of oxo-centered triruthenium(II,III,III) clusters [Ru 3 O(CHCl 2 COO) 6 (py) 3 ] (1) and [Ru 3 O(CHCl 2 COO) 6 (CO)(py) 2 ] (2) (py = pyridine). Dichloroacetate was chosen for its large scattering factor of the Cl atom, and its electron-withdrawing nature results in significant stabilization of the targeted lower-valent Ru 3 II,III,III state in the cluster framework. Multipole analysis revealed that the difference in electron populations between two crystallographically independent Ru centers is small for 1 (Δ = 0.30 e) but large for 2 (Δ = 1.46 e). Remarkable differences between 1 and 2 are also found in their static deformation density maps; substantial local charge depletion was found around the central μ 3 O atom for 1, which is less pronounced for 2. According to the topological characterization of Ru−μ 3 O bonds associated with the bond critical point, bcp, the electron density, ρ bcp , is in the range of 0.79−0.89 e Å −3 , and the total energy density, H bcp , is in the range of −0.21 to −0.05 hartree Å −3 . These findings represent the first charge-density distribution analysis of mixed-valence multinuclear Ru complexes including comparison between 3d and 4d transition-metal systems.

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A pyrazine‐bridged trimer of oxo‐centered triruthenium–carbonyl clusters and the supramolecular assembly built from multiple noncovalent contacts

Cited by 3 publications

References 60 publications

Understanding the Electrochemistry of Ruthenium Complex Thin Films to Guide the Design of Improved Energy Storage Electrodes

Understanding the Electrochemistry of Ruthenium Complex Thin Films to Guide the Design of Improved Energy Storage Electrodes

Oxo-centered trinuclear ruthenium acetates: Structure and applications

Synthetic, Electrochemical, DFT, and Synchrotron X-ray Charge-Density Studies on Oxo-centered Triruthenium Clusters Supported by Electron-Withdrawing Carboxylates

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