Challenges and perspectives of covalent organic frameworks for advanced alkali-metal ion batteries

Xu, Jie; Xu, Yifan; Lai, Chenling; Xia, Tingting; Zhang, Beining; Zhou, Xiaosi

doi:10.1007/s11426-021-1016-6

Cited by 108 publications

(77 citation statements)

References 75 publications

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“…9 Organic molecules containing redox-active groups are usually condensed into a polymer structure with enhanced conductivity and higher stability, such as conducting polymers, [10][11][12][13] metal organic frameworks (MOFs), [14][15][16] and 2D COFs. [17][18][19] Among them, 2D COFs have conjugated p-electron systems along the 2D plane and open channels along the direction of stacking, providing effective transfer paths for both electrons and ions. 18 Moreover, the periodic and denite architecture of 2D COFs facilitates the understanding of structure-property correlation at the atomic level.…”

Section: Introductionmentioning

confidence: 99%

Two-dimensional covalent organic frameworks with p- and bipolar-type redox-active centers for organic high-performance Li-ion battery cathodes

et al. 2022

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Section: Introductionmentioning

confidence: 99%

Two-dimensional covalent organic frameworks with p- and bipolar-type redox-active centers for organic high-performance Li-ion battery cathodes

et al. 2022

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“…Clearly, S@CTFO displays higher capacity retention at an elevated current density that implies higher sulfur utilization of S@CTFO. In comparison with our previous work on porous aromatic frameworks, , the S@CTFO cathode exhibits improved capacity and cycling stability due to the greatly increased heteroatom content. Comparison was also made with the documented results that used CTF materials as the sulfur support for lithium–sulfur batteries in Table S4.…”

Section: Resultsmentioning

confidence: 63%

“…The energy crisis and the severe environmental problems caused by the excessive consumption of fossil fuels have stimulated the pursuit of clean and efficient energy systems. − In the past few decades, the rapid development of portable electronic products, electric vehicles, and large-scale energy storage systems has aroused an intensive demand for high energy density electrochemical energy storage devices. − Lithium–sulfur (Li–S) batteries , have been widely considered as the next-generation energy storage system due to the high theoretical specific capacity, natural abundance, and low cost of sulfur. − However, at present, the practical application of Li–S batteries is still restricted by the following issues: (1) the intrinsic insulating property of sulfur and the reduction intermediates (Li 2 S x , 1 ≤ x ≤ 2), , (2) the large volume expansion of up to 80% that affects the mechanical stability of the active material, (3) the migration of lithium polysulfide intermediates (Li 2 S n , 8 > n > 2) in the organic electrolytes, resulting in the irreversible loss of the active substance and Li anode . These issues hindered the promotion of energy density and cycle stability of sulfur electrodes .…”

Section: Introductionmentioning

confidence: 99%

New Covalent Triazine Framework Rich in Nitrogen and Oxygen as a Host Material for Lithium–Sulfur Batteries

Gao

Jia

Gao

et al. 2021

ACS Appl. Mater. Interfaces

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Lithium–sulfur (Li–S) batteries have been widely considered as the next-generation energy storage system but hindered by the soluble polysulfide intermediate-induced shuttle effect. Doping heteroatoms was confirmed to enhance the affinity of polysulfide and the carbon host, release the shuttle effect, and improve the battery performance. To enhance the Lewis acidity and reinforce the interaction between polysulfide and the carbon skeleton, a novel covalent triazine framework (CTFO) was designed and fabricated by copolymerizing 2,4,6-triphenoxy-s-triazine and 2,4,6-trichloro-1,3,5-triazine through Friedel–Crafts alkylation. Polymerization led to triazine substitution on the para-position of the phenoxy groups of 2,4,6-triphenoxy-triazine and produced two-dimensional three-connected honeycomb nanosheets. These nanosheets were confirmed to exhibit packing in the AB style through the intralayer π–π interaction to form a three-dimensional layered network with micropores of 0.5 nm. The practical and simulated results manifested the enhanced polysulfide capture capability due to the abundant N and O heteroatoms in CTFO. The unique porous polar network endowed CTFO with improved Li–S battery performance with high Coulombic efficiency, rate capability, and cycling stability. The S@CTFO cathode delivered an initial discharge capacity of 791 mAh g–1 at 1C and retained a residual capacity of 512 mAh g–1 after 300 charge–discharge cycles with an attenuation rate of 0.117%. The present results confirmed that multiple heteroatom doping enhances the interaction between the porous polar CTF skeleton and polysulfide intermediates to improve the Li–S battery performance.

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“…As we know, the configurations of N doped in graphitic carbon including pyrrolic N (N-5), quaternary N (N-Q), and pyridinic N (N-6) can be found at defect, edge sites, and skeleton in graphite planes due to the replacement of C atoms with N atoms, respectively. Different from N-Q, N-5 and N-6 are believed to be more active for electrochemical energy storage, depending on the fact that defects and more active sites are induced, and alkali metal ions are more adsorbed in an energy-efficient way. − However, N-doped nanocarbon usually contains a mixture of different nitrogen configurations because of its unstable state under high temperature, it is a rigorous challenge to accurately identify the behavior of a certain configuration of nitrogen on sodium storage to guide the nitrogen doping to further improve the performance of sodium batteries.…”

Section: Introductionmentioning

confidence: 99%

Effect of Different Nitrogen Configurations on Sodium Storage Properties of Carbon Anodes for Sodium Ion Batteries

Feng

Bai

Zheng

et al. 2021

ACS Appl. Mater. Interfaces

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Nitrogen doping carbon materials are considered to be promising candidates for Na+ storage anodes. However, hitherto, the effects and mechanism of specific single N configuration (among pyrrolic N, quaternary N, and pyridinic N), on the sodium storage behaviors of carbon materials, are still puzzling, owing to the difficulties in accurately synthesizing a certain type of single N configuration dominated carbon materials (NCDCMs). Here, various NCDCMs have been successfully controlled and synthesized by small molecule polymerization methods, and their synthesis process has been also verified by NMR, MOLDI-TOF, TG-MS, etc. When serving as sodium ion battery anodes, the NCDCMs dominated by a high concentration of pyrrolic N (>80.3%) exhibits a satisfactory reversible capacity (434.5 mA h g–1 at 50 mA g–1 and 146.7 mA h g–1 at 2000 mA g–1, respectively). It is revealed that pyrrolic N has more suitable adsorption energy and larger interlayer spacing, by density functional theory calculations and electron orbital theory, respectively, which synergistically makes the material obtain excellent electrochemical performance. This research exhibits a more efficient way to reveal the differences in the sodium ions storage behavior of different nitrogen configurations doped carbon, and provides new insight for the precise design and synthesis of a certain type of heteroatom doping to achieve satisfactory electrochemical performance.

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Challenges and perspectives of covalent organic frameworks for advanced alkali-metal ion batteries

Cited by 108 publications

References 75 publications

Two-dimensional covalent organic frameworks with p- and bipolar-type redox-active centers for organic high-performance Li-ion battery cathodes

Two-dimensional covalent organic frameworks with p- and bipolar-type redox-active centers for organic high-performance Li-ion battery cathodes

New Covalent Triazine Framework Rich in Nitrogen and Oxygen as a Host Material for Lithium–Sulfur Batteries

Effect of Different Nitrogen Configurations on Sodium Storage Properties of Carbon Anodes for Sodium Ion Batteries

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