Constructing ambivalent imidazopyridinium-linked covalent organic frameworks

Li, Xing; Zhang, Kun; Wang, Gang; Yuan, Yijia; Zhan, Gaolei; Ghosh, Tanmay; Wong, Walter P. D.; Chen, Fangzheng; Xu, Hai‐Sen; Mirsaidov, Utkur; Xie, Keyu; Lin, Junhao; Loh, Kian Ping

doi:10.1038/s44160-022-00071-y

Cited by 62 publications

(40 citation statements)

References 69 publications

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“…A symmetrical cell with 0.5 mol/L Li 2 S 6 electrolyte and blank aluminum foil electrodes is another control group. CV measurements were conducted on a CHI760E electrochemical workstation at 20 mV/s within −1 to +1 V. , …”

Section: Methodsmentioning

confidence: 99%

“…To meet the ever-increasing requirement for economical and high-efficiency electrical energy-storage devices facilitated by the fast development of power grid and transportation industry, advanced cells with low-cost, long life span, and high-energy density need to be developed. Rechargeable lithium–sulfur batteries (LSBs) are widely regarded as very promising next-generation energy-storage devices with high-energy density (≈2600 Wh/kg or 2800 Wh/L) because of the absolute predominance of sulfur (S) cathode, such as a high theoretical specific capacity ( C s ) of 1672 mAh/g, environmental benignity, low-cost, and natural abundance. − Nevertheless, there are still many hurdles such as the shuttle effect of highly soluble lithium polysulfides (LiPSs), electric insulation nature, and obvious volumetric variation of S, limiting the large-scale application of LSBs. − To enhance LSBs’ performance, many strategies have been proposed to solve these problems, including the construction of advanced S cathode, ,, employing modified adhesives, , adding electrolyte additives, , introducing conductive interlayers, , and using multifunctional separators. , …”

Section: Introductionmentioning

confidence: 99%

“…1−4 Nevertheless, there are still many hurdles such as the shuttle effect of highly soluble lithium polysulfides (LiPSs), electric insulation nature, and obvious volumetric variation of S, limiting the large-scale application of LSBs. 5−7 To enhance LSBs' performance, many strategies have been proposed to solve these problems, including the construction of advanced S cathode, 2,8,9 employing modified adhesives, 10,11 adding electrolyte additives, 12,13 introducing conductive interlayers, 14,15 and using multifunctional separators. 16,17 Except for the electrochemical performance, the safety issue of LSBs also deserves attention in commercial applications due to the presence of highly flammable polymer separators, organic electrolytes, S, and active lithium metal.…”

Section: ■ Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Toward Safe and High-Performance Lithium–Sulfur Batteries via Polyimide Nanosheets-Modified Separator

Zhu

Zhang

Jin

et al. 2023

ACS Sustainable Chem. Eng.

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Lithium−sulfur batteries (LSBs) have broad application prospects in high density energy storage. Nevertheless, LSBs present serious safety concerns and rapid capacity decay due to the flammability and contractility of commercial separators at high temperatures and lithium polysulfide (LiPSs) dissolution. In view of this, a multifunctional modified separator is developed by combining a commercial polypropylene (PP) separator with a polyimide (PI)-Super P functional coating and a rigid nonflammable PI matrix. This PI/PP/PI-Super P separator provides multiple advantages: (i) strong physical blocking and chemical trapping/conversion ability for LiPSs, (ii) high flame-retardancy and dimensional stability, and (iii) superior electrolyte wettability and high efficiency lithium dendritic growth inhibition. As a result, the LSBs assembled with PI/PP/PI-Super P separators and pure sulfur cathodes exhibit an ultrahigh discharge specific capacity of 1611.8 mAh/g and excellent cycling performance (the average capacity attenuation within 100 cycles at 1 C is 0.469%) at 80 °C, which exceed the advanced results reported previously. More importantly, even when sulfur and organic electrolyte are adsorbed on PI/ PP/PI-Super P, the modified separator still shows good flame retardancy. Additionally, this modified separator is also suitable for LSBs with high sulfur loading. This work offers an innovative design concept for safe and high-performance LSBs.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Toward Safe and High-Performance Lithium–Sulfur Batteries via Polyimide Nanosheets-Modified Separator

Zhu

Zhang

Jin

et al. 2023

ACS Sustainable Chem. Eng.

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“…Next-generation rechargeable batteries with high energy density are researched intensely due to rising energy demands of portable electronic devices and electric vehicles. − With current Li-ion battery systems approaching their theoretical energy density limits, lithium–sulfur (Li–S) battery is widely considered as the next-generation high-energy lithium-based battery system due to its high theoretical energy density (2600 W h kg –1 ), low cost, and natural abundance. , Notwithstanding these outstanding qualities, the pernicious “shuttle effect” caused by negatively charged polysulfides dissolving in the ether electrolyte and moving across the separator results in severe capacity fading and electrode destruction during battery operation. , Moreover, the sluggish diffusion of Li ions across commercial PP separators causes dendritic Li formation. These problems present formidable challenges for realizing practical Li–S batteries. , Therefore, it is highly desirable to develop permselective membranes to regulate the migration of cations and anions simultaneously in Li–S batteries.…”

Section: Introductionmentioning

confidence: 99%

Fluorinated Covalent Organic Framework-Based Nanofluidic Interface for Robust Lithium–Sulfur Batteries

Zhang

et al. 2023

ACS Nano

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To realize the practical application of lithium-sulfur (Li-S) batteries, there is a need to inhibit uncontrolled Li deposition by facilitating Li-ion migration, and suppress the irreversible consumption of cathodes by preventing polysulfide shuttling. However, a permselective artifical membrane or interlayer which features fast ion transport but low polysulfide crossover is elusive. Here, we report the design and synthesis of a fluorinated covalent organic framework (4F-COF)-based membrane with a high permselectivity and increased battery lifespan. Combining density functional theory calculation, molecular dynamic simulation, and in situ Raman analysis, we demonstrate that fluorinated COF eliminates polysulfides shutting and dendritic lithium formation. Consequently, Li symmetrical cells demonstrate Li plating/stripping behaviors for 2000 h under 1 mA cm −2 . More importantly, Li−S batteries based on the 4F-COF/PP separator achieve cycling retention of 82.3% over 1000 cycles at 2 C, rate performance of 568.0 mA h g −1 at 10 C, and an areal capacity of 7.60 mA h cm −2 with a high sulfur loading (∼9 mg cm −2 ). This work demonstrates that functionalizing nanochannels in COFs can impart permselectivity for energy storage applications.

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“…Two-dimensional conjugated covalent organic frameworks (2D c-COFs) [14][15][16][17] represent an emerging class of crystalline 2D conjugated polymers with defined porosity [18][19] and active sites [20][21] as well as tailorable electro-activity [22][23][24] , which are promising candidates for electronic 25 and electrochemical [26][27][28][29] applications. In particular, the incorporation of redox-active units would confer unique redox-behavior to the resultant 2D c-COFs.…”

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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Constructing ambivalent imidazopyridinium-linked covalent organic frameworks

Cited by 62 publications

References 69 publications

Toward Safe and High-Performance Lithium–Sulfur Batteries via Polyimide Nanosheets-Modified Separator

Toward Safe and High-Performance Lithium–Sulfur Batteries via Polyimide Nanosheets-Modified Separator

Fluorinated Covalent Organic Framework-Based Nanofluidic Interface for Robust Lithium–Sulfur Batteries

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

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