Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries

Zhao, Chen; Xu, Gui‐Liang; Zhao, Tianshou; Amine, Khalil

doi:10.1002/ange.202007159

Cited by 12 publications

(3 citation statements)

References 47 publications

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“…T he ever-growing demand for high-energy and low-cost batteries has boosted the exploration of novel electrochemistry beyond conventional lithium-ion batteries. Li-S batteries have drawn much attention because of their high theoretical energy density (2600 Wh kg −1 ) and the earth abundance of sulfur resources [1][2][3][4][5][6] . A typical Li-S battery is composed of a Li metal anode and a sulfur cathode, separated by a polypropylene separator and a Li + -conducting organic electrolyte 4,7 .…”

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confidence: 99%

“…The commercialization of Li-S batteries has been hindered by their low practical energy density, poor cycle life, and severe self-discharg [8][9][10] . These drawbacks are directly related to the dissolution/shuttling of long-chain lithium polysulfides (LiPSs) during battery operation [1][2][3][4] . A conventional strategy to mitigate these problems is to immobilize LiPSs within a rational sulfur host via physical/chemical adsorption, such as conductive carbon [11][12][13][14] , polar materials [15][16][17] , or singleatom catalyst [18][19][20] .…”

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confidence: 99%

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Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Lee

Zhao

et al. 2022

Nat Commun

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Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm−2 (for a total sulfur mass loading of 10 mg cm−2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g−1 and 25 °C.

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confidence: 99%

Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Lee

Zhao

et al. 2022

Nat Commun

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“…The rate performances of the batteries were tested at 0.1, 0.2, 0.5, 1.0, and 2.0 C, respectively. At the same time, cyclic voltammetry (CV, 1.5–3.0 V) and electrochemical impedance spectroscopy (EIS; 10 mHz−100 kHz) were performed by Biologic VMP‐3 multichannel workstation 47,78 . All the above electrochemical performance tests were carried out in an incubator at 26°C.…”

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confidence: 99%

Sulfur polymerization strategy based on the intrinsic properties of polymers for advanced binder‐free and high‐sulfur‐content Li–S batteries

Song

Zhang

Liu

et al. 2023

SusMat

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Lithium-sulfur (Li-S) batteries are the promising next-generation secondary energy storage systems, because of their advantages of high energy density and environmental friendliness. Among numerous cathode materials, organosulfur polymer materials have received extensive attentions because of their controllable structure and uniform sulfur distribution. However, the sulfur content of most organosulfur polymer cathodes is limited (S content <60%) due to the addition of large amounts of conductive agents and binders, which adversely affects the energy density of Li-S batteries. Herein, a hyperbranched sulfur-rich polymer based on modified polyethyleneimine (Ath-PEI) named carbon nanotubeentangled poly (allyl-terminated hyperbranched ethyleneimine-random-sulfur) (CNT/Ath-PEI@S) was prepared by sulfur polymerization and used as a Li-S battery cathode. The high intrinsic viscosity of Ath-PEI provided considerable adhesion and avoided the addition of PVDF binder, thereby increasing the sulfur content of cathodes to 75%. Moreover, considering the uniform distribution of elemental sulfur by the polymer, the utilization of sulfur was successfully improved, thus improving the rate capability and discharge capacity of the battery. The binder-free, sulfur-rich polymer cathode exhibited ultra-high initial discharge capacity (1520.7 mAh g −1 at 0.1 C), and high rate capability (804 mAh g −1 at 2.0 C). And cell-level calculations show that the electrode exhibits an initial capacity of 942.3 mAh g −1 electrode , which is much higher than those of conventional sulfur-polymer electrodes reported in the literature.

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Selective Permeable Lithium‐Ion Channels on Lithium Metal for Practical Lithium–Sulfur Pouch Cells

et al. 2021

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Lithium metal batteries are considered a promising candidate for high‐energy‐density energy storage. However, the strong reducibility and high reactivity of lithium lead to low Coulombic efficiency when contacting oxidants, such as lithium polysulfide caused by the serious “shuttle effect” in lithium–sulfur batteries. Herein we design selectively permeable lithium‐ion channels on lithium metal surface, which allow lithium ions to pass through by electrochemical overpotential, while the polysulfides are effectively blocked due to the much larger steric hindrance than lithium ions. The selective permeation of lithium ions through the channels is further elucidated by the molecular simulation and visualization experiment. Consequently, a prolonged cycle life of 75 cycles and high Coulombic efficiency of 99 % are achieved in a practical Li–S pouch cell with limited amounts of lithium and electrolyte, confirming the unique role the selective ion permeation plays in protecting highly reactive alkali metal anodes in working batteries.

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Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries

Cited by 12 publications

References 47 publications

Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Sulfur polymerization strategy based on the intrinsic properties of polymers for advanced binder‐free and high‐sulfur‐content Li–S batteries

Selective Permeable Lithium‐Ion Channels on Lithium Metal for Practical Lithium–Sulfur Pouch Cells

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