A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode

Gao, Hui; Neale, Alex R.; Zhu, Qiang; Bahri, Mounib; Wang, Xue; Yang, Haofan; Xu, Yongjie; Clowes, Rob; Browning, Nigel D.; Little, Marc A.; Hardwick, Laurence J.; Cooper, Andrew I.

doi:10.1021/jacs.2c02196

Cited by 91 publications

(111 citation statements)

References 42 publications

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“…The band at 1542 cm À1 This journal is © The Royal Society of Chemistry 2022 became weak aer activation, and then it recovered aer discharge to À0.6 V vs. Ag/AgCl. This is related to the changes in delocalization and aromatic characteristics of C]C. 51 As shown in Fig. S2, † the phenol structure changed to benzoquinone structure aer activation, and changed back to the phenol structure aer discharge to À0.6 V. The storage mechanism was further studied by X-ray photoelectron spectroscopy (XPS).…”

Section: Resultsmentioning

confidence: 98%

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A covalent organic framework for high-rate aqueous calcium-ion batteries

Zhang

Deng

et al. 2022

J. Mater. Chem. A

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Section: Resultsmentioning

confidence: 98%

“…This is related to the changes in delocalization and aromatic characteristics of CC. 51 As shown in Fig. S2,† the phenol structure changed to benzoquinone structure after activation, and changed back to the phenol structure after discharge to −0.6 V. The storage mechanism was further studied by X-ray photoelectron spectroscopy (XPS).…”

Section: Resultsmentioning

confidence: 99%

A covalent organic framework for high-rate aqueous calcium-ion batteries

Zhang

Deng

et al. 2022

J. Mater. Chem. A

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“…[ 15,45 ] During reverse charging, the characteristic peak of CO recovers. [ 46 ] Therefore, Li + undergoes a highly reversible enolation with the active CO group in the C 6 O 6 molecule to form a lithium enolate group (COLi). These results are in good agreement with the ex situ FT‐IR analysis.…”

Section: Resultsmentioning

confidence: 99%

Eight‐Electron Redox Cyclohexanehexone Anode for High‐Rate High‐Capacity Lithium Storage

Lin

Zhang

et al. 2022

Advanced Energy Materials

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delivery capacity. [1,2] As an essential component of LIBs, anode materials have continuously been one of the hotspots in battery research to boost the energy density and lifespan. To date, inorganic electrode materials have been dominant in battery anodes. [3] However, inorganic anode materials, especially commercial graphite anodes, suffer from limited theoretical capacity (372 mAh g −1 ) and low rate capability due to conventional Li + intercalation/de-intercalation mechanisms, which inevitably restricts the development of high-energy and high-power density LIBs. [4] As an alternative, high-capacity alloying-type anode materials (e.g., Si, Ge, and Sn), especially silicon-carbon composite and silicon monoxide (SiO), have gained extensive attention and achieved initial applications in recent years. [5] However, these novel anode materials still face great challenges in terms of cycling durability and rate performance, mainly caused by drastic volume variation, severe mechanical pulverization, and cumulative growth of solid electrolyte interphase (SEI) layer upon cycling. [6,7] It should be noted that, in addition to the performance bottleneck, the high carbon emission caused by the high-energy synthesis route is also a serious issue that deserves more attention for inorganic anodes.Replacing inorganic anodes with organic electrode materials is an extremely attractive direction for future LIBs. Organic compounds offer significant merits, including structural diversity, processing compatibility, easy recycling/disposal, and low environmental footprint. [8,9] More importantly, organic anode materials endowed abundant redox-active sites may achieve high capacity, and even make it possible to explore the intriguing energy storage mechanisms towards electrochemical process (e.g., superlithiation). [10,11] Among all organic electroactive anode materials, carbonyl (CO) group-based compounds are being explored as the main candidates for LIBs owing to their high theoretical capacity, accessible active sites, easy synthesis, and availability from natural resources. [12][13][14] In particular, cyclohexanehexone (C 6 O 6 ), as a perfect structure composed entirely of six CO groups, can theoretically contribute the largest number of reactive sites and the highest specific capacity when used as an anode material. However, the research of C 6 O 6 as the anode material for LIBs has not been Replacing inorganic anodes with organic electrode materials is an attractive direction for future green Li-ion batteries (LIBs). Carbonyl compounds are being explored as leading anode candidates for organic LIBs. In particular, cyclohexanehexanone (C 6 O 6 ), as a perfect structure composed entirely of six CO groups, can theoretically contribute to the most reactive sites and the highest specific capacity, but has not been used as an anode material so far owing to its high solubility in carbonate-based electrolytes and extremely low electronic conductivity. Herein, C 6 O 6 is first revealed as an ultra-high capacity and high-rate anode ...

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“…[30][31][32] Two major classes of redox-active sites, i.e. pyrazine 33 (derivatives such as phenazine, 34 hexaazatrinaphthalene 35 ) and conjugated carbonyls 36 (e.g., quinone, [37][38] naphthalene diimide [39][40] ) have been successfully integrated into the COF backbone towards highcapacity and stable metal-ion (i.e. Zn 2+ ) storage or metal-/hydrogen-ion (i.e.…”

Section: Introductionmentioning

confidence: 99%

Perinone-Based Ladder-Type Two-Dimensional Conjugated Covalent Organic Framework for Fast Proton Storage

Wang

Chandrasekhar

et al. 2022

Preprint

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Electrochemical proton storage plays an essential role in designing next-generation high-rate energy storage technologies, e.g., aqueous batteries. Two-dimensional conjugated covalent organic frameworks (2D c-COFs) are promising electrode materials, but their competitive proton and metal-ion insertion mechanisms remain elusive, and COF-based proton storage is rarely explored. Here, we report a perinone-based ladder-type 2D c-COF towards fast proton storage in both mild aqueous Zn-ion electrolyte and strong acid. We unveil that the generated C-O- groups via discharge exhibit largely reduced basicity due to the considerable pi-delocalization in perinone, thus affording the 2D c-COF a unique affinity to proton with fast kinetics. As a consequence, the 2D c-COF electrode presents outstanding rate capability up to 200 A g-1 (over 2500C). Our work reports the first example of proton storage among COFs and highlights the great potential of perinone-based 2D c-COF in future energy devices.

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A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode

Cited by 91 publications

References 42 publications

A covalent organic framework for high-rate aqueous calcium-ion batteries

A covalent organic framework for high-rate aqueous calcium-ion batteries

Eight‐Electron Redox Cyclohexanehexone Anode for High‐Rate High‐Capacity Lithium Storage

Perinone-Based Ladder-Type Two-Dimensional Conjugated Covalent Organic Framework for Fast Proton Storage

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