Investigation of the mechanism of metal–organic frameworks preventing polysulfide shuttling from the perspective of composition and structure

Han, Jing; Gao, Shu; Wang, Ruxing; Wang, Kangli; Jiang, Kai; Yan, Jie; Jin, Qianzheng

doi:10.1039/d0ta00533a

Cited by 32 publications

(27 citation statements)

References 46 publications

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“…And the V 2p (Figure 5d) peaks can be divided into two peaks at 513.7 and 516.5 (2p 3/2 ), corresponding to the V 3+ −N and V 5+ −O bonds, respectively [28] . For Zr 3d XPS peaks (Figure 5e), two main peaks with binding energies of 182.6 and 183.4 eV are observed, corresponding to the Zr 3+ ‐N and Zr 4+ −O, respectively [42] . Impressively, all X 3+ −N peak (X=Nb, Mo, Cr, V and Zr) slightly shift to lower binding energies, relating to the strong chemical interaction between HEMN and LIPS that originated from the electron from negative S x 2− (4≤x≤8) to positive X 3+ (X=Nb, Mo, Cr, V and Zr) [25–29,42] .…”

Section: Resultsmentioning

confidence: 99%

“…For Zr 3d XPS peaks (Figure 5e), two main peaks with binding energies of 182.6 and 183.4 eV are observed, corresponding to the Zr 3+ ‐N and Zr 4+ −O, respectively [42] . Impressively, all X 3+ −N peak (X=Nb, Mo, Cr, V and Zr) slightly shift to lower binding energies, relating to the strong chemical interaction between HEMN and LIPS that originated from the electron from negative S x 2− (4≤x≤8) to positive X 3+ (X=Nb, Mo, Cr, V and Zr) [25–29,42] . For five transition metals, Nb, Mo, Cr, V and Zr, the specific negative shift values are 0.51, 0.43, 0.51, 0.49, and 0.57 eV, respectively.…”

Section: Resultsmentioning

confidence: 99%

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Restraining Polysulfide with High‐Entropy Metal Nitride towards Long Cycle Life and High Capacity Li−S Batteries

et al. 2020

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LithiumÀ sulfur (LiÀ S) batteries with ultrahigh theoretical specific capacity (1675 mAh g À 1) have become a research hotpot, which focuses on the solution of shuttle effect of soluble lithium polysulfides (LIPS). Chemical immobilization of LIPS and encapsulation structure of the sulfur cathode are effective strategies to suppress the shuttle effect. Herein, high entropy metal nitride (HEMN) was prepared by mechanochemicalassisted synthesis as an innovative anchor to restrain LIPS via the chemical bonding interaction between HEMN and LIPS. Furthermore, the composite of HEMN and S was encased by graphene (GR) through electrostatic attraction caused by opposite zeta potential, thus as the effective cathode (HEMN/ S@GR) of LiÀ S batteries. HEMN has plentiful active metal sites which can chemically adsorb LIPS, enhancing the cycle life of LiÀ S batteries. Graphene can accelerate surface charge transfer of sulfur cathode to reduce the interface resistance because of its high conductivity. The initial specific capacity of HEMN/S@GR cathode is 1193 mAh g À 1 and still maintains 695 mAh g À 1 after 100 cycles at 0.1 C. When increased to 1.0 C, the initial specific capacity is 556 mAh g À 1 and exhibits remarkable stability in long cycles. This study presents the synergetic effect of HEMN and graphene on LIPS in LiÀ S batteries, which introduces a new application way of high entropy materials in the field of energy storage devices.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Restraining Polysulfide with High‐Entropy Metal Nitride towards Long Cycle Life and High Capacity Li−S Batteries

et al. 2020

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“…Moreover, both physical and chemical adsorption play important roles in inhibiting polysulfide from shuttling through the intergranular channels of the MOF particles. [ 91 ] Recently, the catalytic effect on MOFs based separator has been proved to be effective to improve redox kinetic of polysulfide conversion, which helps to screen polysulfide as well. [ 92 ]…”

Section: Metal‐organic Framework For Sulfur Cathodementioning

confidence: 99%

Tunable Interaction between Metal‐Organic Frameworks and Electroactive Components in Lithium–Sulfur Batteries: Status and Perspectives

Sun

Fan

et al. 2021

Advanced Energy Materials

106

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lithium-ion batteries (LIBs) have proven an unprecedented success in portable electronics, electric vehicles, grid storage, etc., which make a great difference in our lives. Hence, the 2019 Nobel Prize in Chemistry was awarded to John B. Goodenough, M. Stanley Whittingham, and Akira Yoshino for their revolutionary work in the field of LIBs. [1] The current LIBs technology is based on insertion-compound anode and cathode materials. As shown in Figure 1, the capacities of the insertion-oxide cathodes have reached the limit of ≈250 mAh g −1 , and that of the graphite anode is also limited to ≈370 mAh g −1 . However, the limited capacities are unable to satisfy the ever-growing need for gravimetric and volumetric energy density. It is required topic to develop next generation energy technology. Targeting the goal, researchers have their sights set on alternative electrode materials. On the anode side, based on conversion reactions while accommodating more ions and electrons are becoming promising options. [2] Approaching mature silicon/ carbon anode elevates anode capacity well. [3] And lithium metal anode are also booming. [4] On the cathode side, multi-electron conversion reaction represented by sulfur and oxygen electrode can offer capacities exceed that of conventional insertion cathodes, such as, LiCoO 2 and LiMn 2 O 4 , by an order of magnitude (>1500 mAh g −1 ). Since 2009, lithium-sulfur (Li-S) batteries have received increasing attention and are considered as one of the most promising candidates for next-generation rechargeable batteries after the development of high-performance Li-S batteries by CMK-3 as host. [5] Sulfur, as one of the most abundant elements on earth, is an electrochemically active material that can accept two electrons per atom at ≈2.1 V (vs. Li + /Li). [6] As a result, sulfur cathode materials have high theoretical capacity of 1675 mAh g −1 , and Li-S batteries have theoretical energy density of ≈2600 Wh kg −1 . [7] However, the issues including low conductivity of S and Li 2 S, shuttle effect, large volumetric expansion, and unstable lithium metal anode have to face. [8] Up to now, intensive efforts in component regulation and structure engineering electrode materials have been focused on solving these issues.Sulfur cathodes with high sulfur content (>90 wt%), [9] excellent cycling life (>3000 cycles), [10] as well as, high operating Lithium-sulfur (Li-S) batteries, with high theoretical energy density, promise to be the optimal candidate of next-generation energy-storage. Rapid development in materials has made a major step forward in Li-S batteries. However, a big gap in cycle life and efficiency for practical applications still remains. Reasonable design of materials/electrodes a is significant aspect that must be addressed. The rising metal-organic frameworks (MOFs) are a new class of crystalline porous organic-inorganic hybrid materials. Abundant inorganic nodes and designable organic linkers allow tailored pore chemistry at a molecular-scale, which enables tunable interaction w...

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“…To overcome the foregoing drawbacks, extensive strategies have been proposed and great progress has been achieved by designing applicable sulfur hosts, modifying effective separators, making functional interlayers and exploring advanced electrolytes. [11][12][13] Among these studies, the modified separators are simple and effective in reducing the shuttle effect. Generally, some crucial features should be possessed: (1) the thin and light enough, the thick and heavy separator (> 0.3 mg cm À 1 ) will reduce the diffusion of lithium ions, consume more electrolyte and decrease the overall energy density; (2) the excellent conductivity.…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Multifunctional FeP/Spongy Carbon Modified Separator with Enhanced Polysulfide Immobilization and Conversion for Flame‐Retardant Lithium‐Sulfur Batteries

Zhao

Cheng

et al. 2021

ChemistrySelect

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Lithium-sulfur batteries have been deemed as one of the most promising energy storage systems for the next-generation batteries. However, some serious challenges hinder the commercialization, such as the shuttle effect of polysulfides and sluggish redox kinetics. Herein, novel FeP/spongy carbon (SC) composites with multiple adsorptions and catalytic sites are prepared as a modified separator. Specifically, the SC proves the structural stability and long ions/electron transmission channel. The adding of FeP can spontaneously react with polysulfides to block the shuttling and catalyze the conversion of sulfur chemistry. The formed adsorption-diffu-sion-conversion surface is beneficial to reduce the polarization and accelerate the redox kinetics. Furthermore, the FeP/SC modified separator can bring down the flammability to prove high-safety LSBs. Benefiting from these features, the assembled cells with FeP/SC exhibits extraordinary cycling stability (526 mAh g À 1 over 400 cycles at 1 C), a superior rate property with 619 mAh g À 1 at 2 C. Moreover, the cells with a high areal sulfur loading of 4 mg cm À 2 can maintain a capacity of 618 mAh g À 1 after 150 cycles. Such a FeP/SC modified separator provides a potential commercial application for high-safety and advanced Lithium-sulfur batteries.

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Investigation of the mechanism of metal–organic frameworks preventing polysulfide shuttling from the perspective of composition and structure

Abstract: The inhibition of polysulfides by a MOF composite separator with an ion sieve effect, and physical and chemical adsorption is illustrated.

Cited by 32 publications

References 46 publications

Restraining Polysulfide with High‐Entropy Metal Nitride towards Long Cycle Life and High Capacity Li−S Batteries

Restraining Polysulfide with High‐Entropy Metal Nitride towards Long Cycle Life and High Capacity Li−S Batteries

Tunable Interaction between Metal‐Organic Frameworks and Electroactive Components in Lithium–Sulfur Batteries: Status and Perspectives

Multifunctional FeP/Spongy Carbon Modified Separator with Enhanced Polysulfide Immobilization and Conversion for Flame‐Retardant Lithium‐Sulfur Batteries

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