Multielectron‐Transfer‐based Rechargeable Energy Storage of Two‐Dimensional Coordination Frameworks with Non‐Innocent Ligands

Wada, Keisuke; Sakaushi, Ken; Sasaki, Sono; Nishihara, Hiroshi

doi:10.1002/anie.201802521

Cited by 206 publications

(191 citation statements)

References 37 publications

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“…[17] Furthermore, ex situ Fourier transformed infrared (FTIR) spectra recorded at different charge/discharge states provide further evidence for the redox mechanism of the 2D Cu-THQ MOF (Figure 3 b). At oxidized state, a new peak appears at about 832 cm À1 , which could be assigned to PF 6 À anions, [18] indicating that PF 6 À are embedded in the framework of 2D Cu-THQ MOF to maintain the charge balance when Cu I cations are oxidized to Cu II . Furthermore, both oxidized and reduced states show a peak of the C = O band at 1600 cm À1 , confirming the existence of carbonyl groups.…”

Section: Angewandte Chemiementioning

confidence: 99%

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

et al. 2020

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Metal–organic framework cathodes usually exhibit low capacity and poor electrochemical performance for Li‐ion storage owing to intrinsic low conductivity and inferior redox activity. Now a redox‐active 2D copper–benzoquinoid (Cu‐THQ) MOF has been synthesized by a simple solvothermal method. The abundant porosity and intrinsic redox character endow the 2D Cu‐THQ MOF with promising electrochemical activity. Superior performance is achieved as a Li‐ion battery cathode with a high reversible capacity (387 mA h g−1), large specific energy density (775 Wh kg−1), and good cycling stability. The reaction mechanism is unveiled by comprehensive spectroscopic techniques: a three‐electron redox reaction per coordination unit and one‐electron redox reaction per copper ion mechanism is demonstrated. This elucidatory understanding sheds new light on future rational design of high‐performance MOF‐based cathode materials for efficient energy storage and conversion.

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Section: Angewandte Chemiementioning

confidence: 99%

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

et al. 2020

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“…Furthermore, ex situ Fourier transformed infrared (FTIR) spectra recorded at different charge/discharge states provide further evidence for the redox mechanism of the 2D Cu‐THQ MOF (Figure b). At oxidized state, a new peak appears at about 832 cm −1 , which could be assigned to PF 6 − anions, indicating that PF 6 − are embedded in the framework of 2D Cu‐THQ MOF to maintain the charge balance when Cu I cations are oxidized to Cu II . Furthermore, both oxidized and reduced states show a peak of the C=O band at 1600 cm −1 , confirming the existence of carbonyl groups .…”

Section: Figurementioning

confidence: 99%

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

et al. 2020

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“…One class of redox‐active materials that offers high electronic conductivity and tunable electrochemical property is the d‐π conjugated coordination compounds . Among them, metallically‐conductive 2D frameworks have gained considerable efforts as effective materials for field‐effect transistors, supercapacitors, and batteries . Nevertheless, their 1D alternatives, which possess similar repeating units and redox properties are keeping unexplored for electrochemical cells.…”

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confidence: 99%

Nanostructured Metal–Organic Conjugated Coordination Polymers with Ligand Tailoring for Superior Rechargeable Energy Storage

Xie

Cheng

Cao

et al. 2019

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only high specific capacity but also fast charging ability as well as long cycle life. [1] Although lithium-ion batteries (LIBs) currently dominate the rechargeable battery market, the conventional lithiation mechanism purely based on diffusion-controlled process limits the pursuit of high energy storage, particularly at harsh current density conditions. [2] To achieve next generation of promising energy storage systems, rational design of hybrid electrode materials that integrate the capacitor-like non-faradaic effect with the battery-like faradaic behavior is of great interest. [3,4] Meanwhile, the combination of both characteristics requires the electrode architecture that can rapidly deliver sufficient charges in a short given time period. In this respect, nanostructured redox-active materials with large surface areas and multiredox activities are the most potential candidates. [5][6][7][8][9][10][11][12] One class of redox-active materials that offers high electronic conductivity and tunable electrochemical property is the d-π conjugated coordination compounds. [13][14][15][16][17] Among them, metallically-conductive 2D frameworks have gained considerable efforts as effective materials for field-effect transistors, [18] supercapacitors, [19][20][21] and batteries. [22,23] Nevertheless, their 1D alternatives, [24][25][26] which possess similar repeating units and redox properties are keeping unexplored for electrochemical cells. Such linear conjugated coordination polymers, which are often obtained through the coordination of d 8 metal ions and conjugated tetradentate ligands, are able to provide good chemical stability due to their strong intermolecular interactions. [13,14] Moreover, their energy storage capability can be further stimulated through nanoengineering approaches.From the perspective of molecular design, here we present an innovative strategy to attain high performance conjugated co ordination polymers. Prior to the fabrication of electrodes, nanostructured Ni-NH and Ni-S were prepared in the first place. Differing from literature methods on precise control of the metal centers (M = Ni, Co, Cu, etc.), [20,22] we focus on the alteration of the bridging bonds in organic ligands (Figure 1a). By keeping the metal center remain unchanged, our initiative motivation is to improve the energy storage stability by substituting the bridging bond in metal-coordination complex. Inspired by Conjugated coordination polymers have become an emerging category of redoxactive materials. Although recent studies heavily focus on the tailoring of metal centers in the complexes to achieve stable electrochemical performance, the effect on different substitutions of the bridging bonds has rarely been studied. An innovative tailoring strategy is presented toward the enhancement of the capacity storage and the stability of metal-organic conjugated coordination polymers. Two nanostructured d-π conjugated compounds, Ni[C 6 H 2 (NH) 4 ] n (Ni-NH) and Ni[C 6 H 2 (NH) 2 S 2 ] n (Ni-S), are evaluated and demonstrated to exhibit ...

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Multielectron‐Transfer‐based Rechargeable Energy Storage of Two‐Dimensional Coordination Frameworks with Non‐Innocent Ligands

Cited by 206 publications

References 37 publications

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity

Nanostructured Metal–Organic Conjugated Coordination Polymers with Ligand Tailoring for Superior Rechargeable Energy Storage

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