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Route to sustainable lithium-sulfur batteries with high practical capacity through a fluorine free polysulfide catholyte and self-standing Carbon Nanofiber membranes.

ABSTRACT: We report on a new strategy to improve the capacity, reduce the manufacturing costs and increase the sustainability of Lithium-Sulfur (LiS) batteries. It is based on a semi-liquid cathode composed of a Li₂S₈ polysulphide catholyte and a binder-free carbon nanofiber membrane with tailored morphology. The polysulphides in the catholyte have the dual role of active material and providing Li⁺-conduction, i.e. no traditional Li-salt is used in this cell. The cell is able to deliver an areal capacity as high as 7?mAh cm^-2, twice than that of commercial Lithium-ion batteries (LiBs) and 2-4 times higher than that of state-of-the-art LiS cells. In addition, the battery concept has an improved sustainability from a material point of view by being mainly based on sulfur and carbon and being completely fluorine-free, no fluorinated salt or binders are used, and has potential for upscaling and competitive price. The combination of these properties makes the semi-liquid LiS cell here reported a very promising new concept for practical large-scale energy storage applications.

SUBMITTER: Lim DH

PROVIDER: S-EPMC5524792 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Polysulfide Speciation and Migration in Catholyte Lithium-Sulfur Cells.

Project description:Semi-liquid catholyte Lithium-Sulfur (Li-S) cells have shown to be a promising path to realize high energy density energy storage devices. In general, Li-S cells rely on the conversion of elemental sulfur to soluble polysulfide species. In the case of catholyte cells, the active material is added through polysulfide species dissolved in the electrolyte. Herein, we use operando Raman spectroscopy to track the speciation and migration of polysulfides in the catholyte to shed light on the processes taking place. Combined with ex-situ surface and electrochemical analysis we show that the migration of polysulfides is central in order to maximize the performance in terms of capacity (active material utilization) as well as interphase stability on the Li-metal anode during cycling. More specifically we show that using a catholyte where the polysulfides have the dual roles of active material and conducting species, e. g. no traditional Li-salt (such as LiTFSI) is present, results in a higher mobility and faster migration of polysulfides. We also reveal how the formation of long chain polysulfides in the catholyte is delayed during charge as a result of rapid formation and migration of shorter chain species, beneficial for reaching higher capacities. However, the depletion of ionic species during the last stage of charge, due to the conversion to and precipitation of elemental sulfur on the cathode support, results in polarization of the cell before full conversion can be achieved.

| S-EPMC9303647 | biostudies-literature

Long Cycle Life Organic Polysulfide Catholyte for Rechargeable Lithium Batteries.

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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

Cofactor-Assisted Artificial Enzyme with Multiple Li-Bond Networks for Sustainable Polysulfide Conversion in Lithium-Sulfur Batteries.

Project description:Lithium-sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor-assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin on carboxylated carbon nanotubes (CNTs) (i.e., [CNTs-MM-hemin]), is presented to efficiently convert polysulfides. The MM cofactors bind with the hemin artificial enzymes and CNT conductive substrates through FeN5 coordination and/or covalent amide bonds to provide high and durable catalytic activity for polysulfide conversions, while π-π conjugations between hemin and CNTs and multiple Li-bond networks offered by MM endow the cathode with good electronic/Li+ transmission ability. This synergistic mechanism enables rapid sulfur reaction kinetics, alleviated polysulfide shuttling, and an ultralow (<1.3%) loss of hemin active sites in electrolyte, which is ≈60 times lower than those of noncovalent crosslinked samples. As a result, the Li-S battery using [CNTs-MM-hemin] cathode retains a capacity of 571 mAh g-1 after 900 cycles at 1C with an ultralow capacity decay rate of 0.046% per cycle. Even under raising sulfur loadings up to 7.5 mg cm-2 , the cathode still can steadily run 110 cycles with a capacity retention of 83%.

| S-EPMC8787425 | biostudies-literature

Hierarchical TiO2 spheres as highly efficient polysulfide host for lithium-sulfur batteries.

Project description:Hierarchical TiO2 micron spheres assembled by nano-plates were prepared through a facile hydrothermal route. Chemical tuning of the TiO2 through hydrogen reduction (H-TiO2) is shown to increase oxygen-vacancy density and thereby modifies the electronic properties. H-TiO2 spheres with a polar surface serve as the surface-bound intermediates for strong polysulfides binding. Under the restricting and recapturing effect, the sulfur cathode could deliver a high reversible capacity of 928.1?mA h g(-1) after 50 charge-discharge cycles at a current density of 200?mA g(-1). The H-TiO2 additive developed here is practical for restricting and recapturing the polysulfide from the electrolyte.

| S-EPMC4786857 | biostudies-other

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Project description:During the continuous charge and discharge process in lithium-sulfur batteries, one of the next-generation batteries, polysulfides are generated in the battery's electrolyte, and impact its performance in terms of power and capacity by involving the process. The amount of polysulfides in the electrolyte could be estimated by the change of the Gibbs free energy of the electrolyte, [Formula: see text] in the presence of polysulfide. However, obtaining [Formula: see text] of the diverse mixtures of components in the electrolyte is a complex and expensive task that shows itself as a bottleneck in optimization of electrolytes. In this work, we present a machine-learning approach for predicting [Formula: see text] of electrolytes. The proposed architecture utilizes (1) an attention-based model (Attentive FP), a contrastive learning model (MolCLR) or morgan fingerprints to represent chemical components, and (2) transformers to account for the interactions between chemicals in the electrolyte. This architecture was not only capable of predicting electrolyte properties, including those of chemicals not used during training, but also providing insights into chemical interactions within electrolytes. It revealed that interactions with other chemicals relate to the logP and molecular weight of the chemicals.

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| S-EPMC6765254 | biostudies-literature

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