Inhibition of Polysulfide Shuttles in Li–S Batteries: Modified Separators and Solid‐State Electrolytes

Li, Shulian; Zhang, Weifeng; Zheng, Jiafen; Lv, Mengyuan; Song, Huiyu; Du, Li

doi:10.1002/aenm.202000779

Cited by 225 publications

(168 citation statements)

References 226 publications

(245 reference statements)

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“…Figure 2 c depicts the charge/discharge voltage profiles of the PEO/LiTFSI-coated polypropylene membrane; it features overlapping discharge and charge curves over 200 continuous cycles, suggesting improved capacity retention. This high electrochemical stability indicates that the PEO/LiTFSI coating stabilizes the dissolved polysulfides within the cathode region of the cell [ 10 , 41 ]. The enhanced electrochemical efficiency and reversibility suggests that the coated PEO/LiTFSI film functions as a gel polymer electrolyte that ensures smooth lithium-ion transfer and hence a long cycle life with low polarization ( Figure S3 ).…”

Section: Resultsmentioning

confidence: 99%

A Poly(ethylene oxide)/Lithium bis(trifluoromethanesulfonyl)imide-Coated Polypropylene Membrane for a High-Loading Lithium–Sulfur Battery

Chiu

Chung

2021

Polymers

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In lithium–sulfur cells, the dissolution and relocation of the liquid-state active material (polysulfides) lead to fast capacity fading and low Coulombic efficiency, resulting in poor long-term electrochemical stability. To solve this problem, we synthesize a composite using a gel polymer electrolyte and a separator as a functional membrane, coated with a layer of poly(ethylene oxide) (PEO) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The PEO/LiTFSI-coated polypropylene membrane slows the diffusion of polysulfides and stabilizes the liquid-state active material within the cathode region of the cell, while allowing smooth lithium-ion transfer. The lithium-sulfur cells with the developed membrane demonstrate a high charge-storage capacity of 1212 mA∙h g−1, 981 mA∙h g−1, and 637 mA∙h g−1 at high sulfur loadings of 2 mg cm−2, 4 mg cm−2, and 6 mg cm−2, respectively, and maintains a high reversible capacity of 534 mA∙h g−1 after 200 cycles, proving its ability to block the irreversible diffusion of polysulfides and to maintain the stabilized polysulfides as the catholyte for improved electrochemical utilization and stability. As a comparison, reference and control cells fabricated using a PEO-coated polypropylene membrane and a regular separator, respectively, show a poor capacity of 662 mA∙h g−1 and a short cycle life of 50 cycles.

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Section: Resultsmentioning

confidence: 99%

A Poly(ethylene oxide)/Lithium bis(trifluoromethanesulfonyl)imide-Coated Polypropylene Membrane for a High-Loading Lithium–Sulfur Battery

Chiu

Chung

2021

Polymers

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“…However, to design these matrixes usually need complex fabrication process, which will increase the cost and reduce the whole energy density. Another solution is electrolyte modification, including exploring solid‐state electrolyte and adding additives [64–66] . In particular, ionic liquid‐based electrolytes were widely studied in Li−S batteries because their relatively weak Lewis acidity/basicity could suppress the dissolution of polysulfides in electrolytes [67] .…”

Section: Ionic Liquids For Lithium Sulfur Batteriesmentioning

confidence: 99%

Roadmap on Ionic Liquid Electrolytes for Energy Storage Devices

Yang

et al. 2021

Chemistry An Asian Journal

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Ionic liquids are considered to be promising electrolyte solvents or additives for rechargeable batteries (i. e., lithium‐ion batteries, sodium‐ion batteries, lithium‐sulfur batteries, aluminum‐ion batteries, etc.) and supercapacitors. This is related with the superior physical and electrochemical properties of ionic liquids, which can influence the performance of rechargeable batteries. Therefore, it is necessary to write a roadmap on ionic liquids for rechargeable batteries. In this roadmap, some progress, critical techniques, opportunities and challenges of ionic liquid electrolytes for various batteries and supercapacitors are pointed out. Especially, properties and roles of ionic liquids should be considered in energy storage. Ionic liquids can be used as electrolyte salts, electrolyte additives, and solvents. For optimizing ionic liquid‐based electrolytes for energy storage, their applications in various energy storage devices should be considered by combing native chemical/physical properties and their roles. We expect that this roadmap will give a useful guidance in directing future research in ionic liquid electrolytes for rechargeable batteries and supercapacitors.

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“…However, due to the low ionic conductivity of solids and the unstable cathode/solid electrolyte interface, their rate and cycling performance need to improve. [ 180 ] Han et al., [ 181 ] fabricated a novel class of all‐solid‐state LSBs based on the Li 7 P 3 S 11 glass‐ceramic solid electrolyte (σ = 2.0 and 5.2 × 10 −3 S cm −1 at RT and 80 °C, respectively) and a sulfur/carbon nanocomposite cathode (S@BP2000). The core‐shell structure of S@BP2000 can improve the electrical conductivity, decrease the ohmic polarization, and accommodate the volume expansion of the electrode during cycling.…”

Section: Solid‐state Electrolytesmentioning

confidence: 99%

Rechargeable Battery Electrolytes Capable of Operating over Wide Temperature Windows and Delivering High Safety

Lin

Zhou

Liu

et al. 2020

Advanced Energy Materials

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self-discharge rates. [1-3] LIBs permeate nearly every aspect of human life. They are widely used in portable electronics (e.g., smartphones, smart-watches, and laptops), transportation (e.g., electric and hybrid vehicles), and biomedical applications (e.g., cardiac pacemakers and cochlear implants). In light of these achievements, J.B. Goodenough, M.S. Whittingham, and A. Yoshino won the 2019 Nobel prize in chemistry. [4] Despite the considerable success of conventional LIBs, their operational regime is typically around room temperature (RT). Operating at low (<0 °C) or high (>60 °C) temperatures usually deteriorate the performance and leads to safety risks. [5] We should also note that commercial LIBs are highly hazardous as they can ignite and explode in case of an accident, overheating, and overcharging, requiring more stringent safety standards, e.g., wide temperature operability and nonflammability. For example, electric vehicles require battery systems that can deliver a stable performance while maintaining a high energy density even in extreme climates, such as cold mountainous areas, where the temperatures can be as low as −40 °C, and hot deserts, where equipment exposed to sunlight can reach temperatures exceeding 70 °C. [6] Moreover, task-specific applications call for reliable energy storage solutions at extreme temperatures, including subsurface exploration (such as for mineral, oil, and gas), aerospace engineering, safety and rescue, and sterilizable medical devices. [2] Conventional LIBs are composed of a positive electrode or cathode (e.g., LiFePO 4 (LFP), LiNi x Mn y Co z O 2 (x + y + z = 1, NMC) and LiCoO 2 (LCO)), an electrolyte (including solvents, Li salts, and additives), a separator (typically a polyolefin membrane), and a negative electrode or anode (e.g., graphite and Li 4 Ti 5 O 12 (LTO)). Generally, the electrode materials are nonflammable and thermal stable (>300 °C). While the polyolefin membrane will melt/shrink over 120 °C, the commercial separators composited with ceramic nanoparticle (e.g., SiO 2 and Al 2 O 3) have been developed to reduce thermal shrinkage when exposed to overheating. [7,8] Therefore, the major challenge of commercial LIBs at extreme operating temperatures comes to the electrolyte. Carbonates are commonly used as solvents for conventional LIB electrolytes. However, these compounds are Li-ion batteries (LIBs) are the energy storage systems of choice for portable electronics and electric vehicles. Due to the growing deployment of energy storage solutions, LIBs are increasingly required to function safely and steadily over a broad range of operational conditions. However, the conventional electrolytes used in LIBs will malfunction when the temperatures fall below zero or elevate above 60 °C. Further, conventional electrolytes are toxic and flammable, leading to severe safety risks, especially in the case of an accident or overheating. Therefore, an ever-growing body of research has been dedicated to the development of electrolytes characterized by high ionic conduct...

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Inhibition of Polysulfide Shuttles in Li–S Batteries: Modified Separators and Solid‐State Electrolytes

Cited by 225 publications

References 226 publications

A Poly(ethylene oxide)/Lithium bis(trifluoromethanesulfonyl)imide-Coated Polypropylene Membrane for a High-Loading Lithium–Sulfur Battery

A Poly(ethylene oxide)/Lithium bis(trifluoromethanesulfonyl)imide-Coated Polypropylene Membrane for a High-Loading Lithium–Sulfur Battery

Roadmap on Ionic Liquid Electrolytes for Energy Storage Devices

Rechargeable Battery Electrolytes Capable of Operating over Wide Temperature Windows and Delivering High Safety

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