A robust electrospun separator modified with in situ grown metal-organic frameworks for lithium-sulfur batteries

Zhou, Cheng; He, Qiu; Li, Zhaohuai; Meng, Jiashen; Hong, Xufeng; Li, Yan; Zhao, Yan; Xu, Xu; Mai, Liqiang

doi:10.1016/j.cej.2020.124979

Cited by 99 publications

(55 citation statements)

References 52 publications

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“…Since adsorption is the first step in catalysis, the calculated binding energies of adsorption can be used to interpret the affinity for different polysulfide intermediates. There are bifunctional modes for the interaction between MOFs and the polysulfides due to electronegativity differences, [49] where Li + ions bind with O atoms and S n 2− prefer to interact with cobalt or nickel metal centers (Figures S14 and S15, Supporting Information), respectively. The calculated binding energies of the long polysulfides (Li 2 S 8 , Li 2 S 6 , and Li 2 S 4 ) with Ni-MOF are higher than that of the Co-MOF, whereas the binding energies of the short sulfur species (Li 2 S and Li 2 S 2 ) with the Co-MOF are higher than that of the Ni-MOF (Figure 5a).…”

Section: Thermodynamically Understand the Catalytical Discrepanciesmentioning

confidence: 99%

A Tandem Electrocatalysis of Sulfur Reduction by Bimetal 2D MOFs

Meng

Zhong

et al. 2021

Advanced Energy Materials

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polysulfide by the host materials are conventional approaches to tackle the dissolution problem, [3,4] nonetheless, these could only partially alleviate the shuttle effect due to low fraction of host material in the electrode. Using "flooded" electrolyte could dilute the polysulfide solution thus somehow improves the redox kinetics due to enhanced mass/charge transfer, although it inevitably decreases the actual energy density of the battery. [1] Alternatively, recently established proactive electrocatalysis strategy could not only effectively improve the redox kinetics but also provide a "root" solution to solve the polysulfide shuttling. [5,6] The catalyzed sulfur redox reaction showed faster conversion kinetics, especially for the conversion of soluble LiPSs into the insoluble final products, thus preventing the continuous accumulation of LiPSs in electrolyte that is responsible for the shuttle effect. [7,8] An increasing number of electrocatalysts have been applied to Li-S batteries, [5,[9][10][11][12] however, systematic study on the kinetic and underlying basis to evaluate the exact role of catalyst addressing the PS shuttling issues is still overlooked. The classic electrocatalysis process is mostly referred to as heterogeneous catalytic reaction [13] -catalyzing a specific reaction instead of a series of reactions-as exemplified by the wellestablished electrocatalysis in fuel cells and water splitting such as the oxygen reduction reaction, oxygen evolution reaction (OER), and hydrogen evolution reaction. [14,15] The electrolysis of sulfur reduction reaction is much more complicated due to the consecutive multistep reduction reaction of sulfur, which brought huge challenge for the design of catalyst. [16] The diversified intermediate products of sulfur species would dynamically disproportionate or centralize in the electrolyte solution. [17] Moreover, one specific sulfur intermediate acts as both the reactant and product for the adjacent consecutive reductions, indicating that the sulfur species in the electrocatalysis reactions are highly conjugated and coupled. In addition to the multistep conversion reactions, the sulfur conversion reaction also involves multiphase transition because the long-chain polysulfides (Li 2 S x , 4 ≤ x ≤ 8) are soluble whereas the shortchain polysulfides (Li 2 S x , 1 ≤ x ≤ 2) is insoluble in the electrolyte. [18] Only a few catalysis works have paid attention to such complicated conversion reactions but mostly focused on the The diversity and coupling of sulfur redox intermediates and its associated solid-liquid-solid multiphase conversion mechanism pose great challenges in designing a proper electrocatalysts for Li-S batteries. In this report, it is proposed that an ideal catalyst should possess two catalytic centers which catalyze liquid-liquid conversion and liquid-solid conversion in tandem within one structure, with the use of 2D MOF nanosheets with different metal centers for validation. It is uncovered that the Ni-MOF is more effective in catalyzing the reduction of lo...

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Section: Thermodynamically Understand the Catalytical Discrepanciesmentioning

confidence: 99%

A Tandem Electrocatalysis of Sulfur Reduction by Bimetal 2D MOFs

Meng

Zhong

et al. 2021

Advanced Energy Materials

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“…As displayed in Table S2, most nanofibrous separators demonstrated a monotone function of suppressing the shuttle effect without protecting Li metal. Although there emerges a study [38] on using the nanofibrous separator to protect Li metal, our Janus separator shows a better performance in terms of the longer cycle life. In other words, the Janus separator from our study proposes an innovative separator design to simultaneously addressing the two critical issues of LiÀ S batteries, that is, shuttle effect and Li dendrite growth.…”

Section: Resultsmentioning

confidence: 92%

A Protein‐Based Janus Separator for Trapping Polysulfides and Regulating Ion Transport in Lithium−Sulfur Batteries

Chen

Liu

et al. 2021

ChemSusChem

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LithiumÀ sulfur (LiÀ S) batteries are a promising candidate for the next-generation energy storage system, yet their commercialization is primarily hindered by polysulfide shuttling and uncontrollable Li dendrite growth. Here, a protein-based Janus separator was designed and fabricated for suppressing both the shuttle effect and dendrite growth, while facilitating the Li + transport. The Li metal-protecting layer was a protein/MoS 2 nanofabric with high ionic conductivity and good Li + affinity, thus capable of homogenizing the Li + flux and facilitating the Li + transport. The polysulfide-trapping layer was a conductive protein nanofabric enabling strong chemical/electrostatic interactions with polysulfides. Combination of the two layers was achieved by an integrated electrospinning method, yielding a robust and integral Janus separator. As a result, a long-lived symmetric Li j Li cell (> 700 h) with stable cycling performance was demonstrated. More significantly, the resulting LiÀ S battery delivered greatly improved electrochemical performance, including excellent rate capacity and remarkable cycle stability (with a low decay rate of 0.063 % per cycle at 0.5 A g À 1 over 500 cycles). This study demonstrates the effectiveness of the Janus separator configurations for simultaneously addressing the shuttle effect and dendrite growth issues of LiÀ S batteries and broadens the applications of electrospinning in electrochemistry community.

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“…reported a double‐layer nanofiber membrane to replace them. [ 112 ] The main material of the membrane was polyacrylonitrile (PAN), where a cobalt‐based MOF and rGO were located on both sides by in situ growth. Figure 12b exhibits the formation process of the MOF–PAN/rGO–PAN separator.…”

Section: The Application Of Mofs In the Separator Of Lsbsmentioning

confidence: 99%

“…Considering that the commercial polyolefin separators commonly used in LSBs have poor mechanical properties and are not resistant to high temperatures, Zhou et al reported a double-layer nanofiber membrane to replace them. [112] The main material of the membrane was polyacrylonitrile (PAN), where a cobalt-based MOF and rGO were located on both sides by in situ growth. Figure 12b exhibits the formation process of the MOF-PAN/rGO-PAN separator.…”

Section: Composite With Graphenementioning

confidence: 99%

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Multifunctional MOF‐Based Separator Materials for Advanced Lithium–Sulfur Batteries

Yuan

Sun

Yang

et al. 2021

Adv Materials Inter

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Despite the high theoretical specific capacity of 1675 mAh g−1, lithium–sulfur batteries (LSBs) are still far away from wide commercialization due to the poor sulfur/Li2S electroconductivity and the polysulfides shuttle effect. In order to alleviate the active materials shuttling, separators in LSBs are required to guarantee the fast lithium‐ion transfer as well as the strong polysulfides immobilization. Therefore, various functional materials have been employed to modify the separator to achieve this goal. Among them, metal–organic frameworks (MOFs) with easy morphology design and high ionic or electronic conductivity have been widely investigated. This review summarizes the recent advances of MOF‐based interlayer for LSBs separator functionalization. Original MOFs, MOF derivatives, and MOF composites are included in this discussion. The mechanism of the enhancement of the electrochemical performance of each modified separator is explicated. Furthermore, the prospect of this promising area is provided.

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A robust electrospun separator modified with in situ grown metal-organic frameworks for lithium-sulfur batteries

Cited by 99 publications

References 52 publications

A Tandem Electrocatalysis of Sulfur Reduction by Bimetal 2D MOFs

A Tandem Electrocatalysis of Sulfur Reduction by Bimetal 2D MOFs

A Protein‐Based Janus Separator for Trapping Polysulfides and Regulating Ion Transport in Lithium−Sulfur Batteries

Multifunctional MOF‐Based Separator Materials for Advanced Lithium–Sulfur Batteries

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