High‐Rate Organic Cathode Constructed by Iron‐Hexaazatrinaphthalene Tricarboxylic Acid Coordination Polymer for Li‐Ion Batteries

Wang, Yifan; Qiao, Zelong; Liu, Kexin; Yu, Le; Lv, Yingying; Shi, Liyi; Zhao, Yin; Cao, Dapeng; Wang, Zhuyi; Wang, Shitao; Yuan, Shuai

doi:10.1002/advs.202205069

Cited by 16 publications

(3 citation statements)

References 58 publications

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“…[23] At low relative pressures, the absorption of N 2 by PSi increases drastically, providing corroboration for the existence of micropores in PSi-1, PSi-2, and PSi-3. [24] The relatively large SSA, high pore volume, and the hierarchical porous structure of PSi-1 enable electrolytes to be in adequate contact with the electrode, which is desirable for reducing ion transport distance, [25] thus contributing to good electrochemical performance.…”

Section: Resultsmentioning

confidence: 99%

Mg‐Doped Porous Silicon Derived from Silica Aerogels for Fast and Stable Zinc‐Ion Hybrid Capacitors with High Capacitance

Deng,

Li,

Zewdie

et al. 2023

Adv Funct Materials

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Zinc‐ion hybrid capacitors (ZICs) are of interest for their optimal balance between power and energy density. Among the cathode materials, silicon is particularly attractive due to its abundance and potential compatibility with the microelectronics industry. However, silicon‐based materials exhibit specific capacitances far below 100 mF cm−2 because of their inherently low electronic and ionic transport, making them less competitive than other nanomaterials such as carbon and MXenes. In this study, state‐of‐the‐art silicon‐based ZICs using Mg‐doped porous silicon (PSi) derived from silica aerogels are constructed. The improved electronic conductivity achieved by Mg doping, combined with enhanced ion diffusion promoted by the porous structure, results in excellent electrochemical properties of the ZIC. Consequently, the prepared ZIC exhibits a specific capacitance of 106.1 mF cm−2 at 0.2 mA cm−2 with remarkable cyclic stability (92% retention after 20 000 cycles). Additionally, the pouch ZICs using gel electrolytes demonstrate good rate capability and a long lifespan, indicating significant potential for practical applications. These results underscore the potential of heteroatom‐doped PSi as a cathode for ZICs.

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Section: Resultsmentioning

confidence: 99%

Mg‐Doped Porous Silicon Derived from Silica Aerogels for Fast and Stable Zinc‐Ion Hybrid Capacitors with High Capacitance

Deng,

Li,

Zewdie

et al. 2023

Adv Funct Materials

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“…Another representative of these materials with abundant active centers is hexaazatriphenylene (HAT) and its derivatives. The unique topological structure of HAT makes it possible to chelate with metal ions by adjacent N or O atoms in HAT units. , Compared with other imine compounds, such as Schiff bases and pyrazine derivatives, the chelation effect of HAT benefits the storage of large-sized alkali metal ions with high capacity and stability. The polymer (HAT-PPDA) based on hexaazatriphenylene imide showed universality as the negative electrode for Li/Na/K ion batteries .…”

Section: Chelation By Electrochemical Active Groupsmentioning

confidence: 99%

Constructing Chelation for Boosting Storage of Large-Sized or Multivalent Ions

Guan,

Zou,

Mao

et al. 2024

Acc. Mater. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: Rechargeable lithium-ion batteries (LIBs) are currently the most popular energy storage devices. However, the essential elements for commercial LIBs, i.e., lithium, cobalt, and nickel, are scarce, leading to an increase in cost, which together with the environmental concerns results in concern for future energy storage and calls for large-scale post-LIBs, including Na-, K-, Ca-, Mg-, Zn-, Al-, and dual-ion batteries. However, these post-LIBs are facing challenges in storage of either large-sized (Na-, K-, Ca-ions, anions) or highcharge-density multivalent (Ca-, Mg-, Zn-, Al-) metal ions. The large ionic sizes will inevitably result in the sluggish ionic diffusion, difficulty in storage, enormous volume variation, pulverization, low capacity, and poor cyclability. While the high charge/radius ratio of multivalent ions leads to strong electrostatic interactions with solvent molecules and electrode lattice, strong solvation, high desolvation energy, possible storage of complex ions, sluggish ionic diffusion and reaction kinetics, low actual capacity, and poor rate capability and cyclability.From this point of view, redox-active organic electrode materials (OEMs) are promising for these post-LIBs. OEMs can be easily synthesized from natural resources, which could meet the low-cost requirements for large-scale applications. Another advantage of OEMs is that the electrochemical performance could be facilely tuned through molecular design. High specific capacity could be expected, surpassing inorganic materials with intercalation chemistry. More importantly, organic materials have the merits of flexibility, which makes it intriguing for storage of large-sized ions with fast kinetics, and relatively small volume variation compared with inorganic electrode materials. In addition, organic/polymeric materials are composed by molecules via weak intermolecular interactions and hence should be suitable for storage of multivalent metal ions with reduced electrostatic interactions. In the past two decades, various OEMs have been reported with decent electrochemical performance for both LIBs and post-LIBs. However, they are still facing a lot of challenges, and effective strategies to enhance the performance of organic batteries are scarce.In the past few years, it has also been found that the storage of ions may lead to chelation with the OEMs when the OEMs have multiple active sites for improving the theoretical capacity or substituents for enhancing the intermolecular interactions. Later, we found that the intentional design of adjacent functional groups for chelation could enhance the storage of ions. In this Account, we first give an overview of challenges faced by post-LIBs and then propose a strategy to boost the storage of large-sized or multivalent metal ions by promoting chelation with stored ions, based on the recent works from our group and others. The findings on chelation with both Li ions and other monovalent and multivalent metal ions are summarized. We hope this A...

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“…However, the resistance of EFID and FBND is still larger than that of high-rate organic materials, [55,57] indicating that this is another factor to be addressed in future studies to improve the rate ability of the active material.…”

Section: Electrochemical Performance Of the Isomers (Efid And Fbnd)mentioning

confidence: 99%

Long Cycle Life for Rechargeable Lithium Battery using Organic Small Molecule Dihydrodibenzo[c,h][2,6]naphthyridine‐5,11‐dione as a Cathode after Isoindigo Pigment Isomerization

Yang,

Hu,

et al. 2023

Advanced Science

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Sustainability and adaptability in structural design of the organic cathodes present promises for applications in alkali metal ion batteries. Nevertheless, a formidable challenge lies in their high solubility in organic electrolytes, particularly for small molecular materials, impeding cycling stability and high capacity. This study focuses on the design and synthesis of organic small molecules, the isomers of (E)‐5,5′‐difluoro‐[3,3′‐biindolinylidene]‐2,2′‐dione (EFID) and 3,9‐difluoro‐6,12‐dihydrodibenzo [c, h][2,6]naphthyridine‐5,11‐dione (FBND). While EFID, characterized by a less π‐conjugated structure, exhibits subpar cycling stability in lithium‐ion batteries (LIBs), intriguingly, another isomer, FBND, demonstrates exceptional capacity and cycling stability in LIBs. FBND delivers a remarkable capacity of 175 mAh g−1 at a current density of 0.05 A g−1 and maintains excellent cycling stability over 2000 cycles, retaining 90% of its initial capacity. Furthermore, an in‐depth examination of redox reactions and storage mechanisms of FBND are conducted. The potential of FBND is also explored as an anode in lithium‐ion batteries (LIBs) and as a cathode in sodium‐ion batteries (SIBs). The FBND framework, featuring extended π‐conjugated molecules with an imide structure compared to EFID, proves to be an excellent material template to develop advanced organic small molecular cathode materials for sustainable batteries.

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High‐Rate Organic Cathode Constructed by Iron‐Hexaazatrinaphthalene Tricarboxylic Acid Coordination Polymer for Li‐Ion Batteries

Cited by 16 publications

References 58 publications

Mg‐Doped Porous Silicon Derived from Silica Aerogels for Fast and Stable Zinc‐Ion Hybrid Capacitors with High Capacitance

Mg‐Doped Porous Silicon Derived from Silica Aerogels for Fast and Stable Zinc‐Ion Hybrid Capacitors with High Capacitance

Constructing Chelation for Boosting Storage of Large-Sized or Multivalent Ions

Long Cycle Life for Rechargeable Lithium Battery using Organic Small Molecule Dihydrodibenzo[c,h][2,6]naphthyridine‐5,11‐dione as a Cathode after Isoindigo Pigment Isomerization

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