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A novel quasi-solid state electrolyte with highly effective polysulfide diffusion inhibition for lithium-sulfur batteries.

ABSTRACT: Polymer solid state electrolytes are actively sought for their potential application in energy storage devices, particularly lithium metal rechargeable batteries. Herein, we report a polymer with high concentration salts as a quasi-solid state electrolyte used for lithium-sulfur cells, which shows an ionic conductivity of 1.6 mS cm(-1) at room temperature. The cycling performance of Li-S battery with this electrolyte shows a long cycle life (300 cycles) and high coulombic efficiency (>98%), without any consuming additives in the electrolyte. Moreover, it also shows a remarkably decreased self-discharge (only 0.2%) after storage for two weeks at room temperature. The reason can be attributed to that the electrolyte can suppress polysulfide anions diffusion, due to the high ratio oxygen atoms with negative charges which induce an electrical repulsion to the polysulfide anions, and their relatively long chains which can provide additional steric hindrance. Thus, the polysulfide anions can be located around carbon particles, which result in remarkably improved overall electrochemical performance, and also the electrolyte have a function of suppress the formation of lithium dendrites on the lithium anode surface.

SUBMITTER: Zhong H

PROVIDER: S-EPMC4857097 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Chloride-Reinforced Carbon Nanofiber Host as Effective Polysulfide Traps in Lithium-Sulfur Batteries.

Project description:Lithium-sulfur (Li-S) battery is one of the most promising alternatives for the current state-of-the-art lithium-ion batteries due to its high theoretical energy density and low production cost from the use of sulfur. However, the commercialization of Li-S batteries has been so far limited to the cyclability and the retention of active sulfur materials. Using co-electrospinning and physical vapor deposition procedures, we created a class of chloride-carbon nanofiber composites, and studied their effectiveness on polysulfides sequestration. By trapping sulfur reduction products in the modified cathode through both chemical and physical confinements, these chloride-coated cathodes are shown to remarkably suppress the polysulfide dissolution and shuttling between lithium and sulfur electrodes. From adsorption experiments and theoretical calculations, it is shown that not only the sulfide-adsorption effect but also the diffusivity in the vicinity of these chlorides materials plays an important role on the reversibility of sulfur-based cathode upon repeated cycles. Balancing the adsorption and diffusion effects of these nonconductive materials could lead to the enhanced cycling performance of an Li-S cell. Electrochemical analyses over hundreds of cycles indicate that cells containing indium chloride-modified carbon nanofiber outperform cells with other halogenated salts, delivering an average specific capacity of above 1200 mAh g-1 at 0.2 C.

| S-EPMC5157171 | biostudies-literature

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Organosulfide-plasticized solid-electrolyte interphase layer enables stable lithium metal anodes for long-cycle lithium-sulfur batteries.

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Project description:The electrochemistry of lithium-sulfur (Li-S) batteries is heavily reliant on the structure and dynamics of lithium polysulfides, which dissolve into the liquid electrolyte and mediate the electrochemical conversion process during operation. This behavior is considerably distinct from the widely used lithium-ion batteries, necessitating new mechanistic insights to fully understand the electrochemical phenomena. Testing at low-temperature conditions presents a unique opportunity to glean new insights into the chemistry in kinetically constrained environments. Under such conditions, despite the low freezing point and favorable ionic conductivity of the glyme-based electrolyte, Li-S batteries exhibit counterintuitively poor performance. Here, we show that beyond just existing in single-molecule conformations, lithium polysulfides tend to cluster and aggregate in solution, particularly at low-temperature conditions, which subsequently constrains the kinetics of electrochemical conversion. Energetics and coordination implications of this behavior are extended towards a new framework for understanding the solution-coordination dynamics of dissolved lithium species. Based off this framework, a favorable strongly-bound lithium salt is introduced in the Li-S electrolyte to disrupt polysulfide clustered networks, enabling substantially enhanced low-temperature electrochemical performance. More broadly, this mechanistic insight heightens our understanding of polysulfide chemistry irrespective of temperature, confirming the link between the solution conformation of active material and electrochemical behavior.

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Multifunctional Sandwich-Structured Electrolyte for High-Performance Lithium-Sulfur Batteries.

Project description:Due to its high theoretical energy density (2600 Wh kg-1), low cost, and environmental benignity, the lithium-sulfur (Li-S) battery is attracting strong interest among the various electrochemical energy storage systems. However, its practical application is seriously hampered by the so-called shuttle effect of the highly soluble polysulfides. Herein, a novel design of multifunctional sandwich-structured polymer electrolyte (polymer/cellulose nonwoven/nanocarbon) for high-performance Li-S batteries is demonstrated. It is verified that Li-S battery with this sandwich-structured polymer electrolyte delivers excellent cycling stability (only 0.039% capacity decay cycle-1 on average exceeding 1500 cycles at 0.5 C) and rate capability (with a reversible capacity of 594 mA h g-1 at 4 C). These electrochemical performances are attributed to the synergistic effect of each layer in this unique sandwich-structured polymer electrolyte including steady lithium stripping/plating, strong polysulfide absorption ability, and increased redox reaction sites. More importantly, even with high sulfur loading of 4.9 mg cm-2, Li-S battery with this sandwich-structured polymer electrolyte can deliver high initial areal capacity of 5.1 mA h cm-2. This demonstrated strategy here may open up a new era of designing hierarchical structured polymer electrolytes for high-performance Li-S batteries.

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| S-EPMC5384807 | biostudies-literature

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