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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.

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| 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

Fluorine-free water-in-ionomer electrolytes for sustainable lithium-ion batteries.

Project description:The continuously increasing number and size of lithium-based batteries developed for large-scale applications raise serious environmental concerns. Herein, we address the issues related to electrolyte toxicity and safety by proposing a "water-in-ionomer" type of electrolyte which replaces organic solvents by water and expensive and toxic fluorinated lithium salts by a non-fluorinated, inexpensive and non-toxic superabsorbing ionomer, lithium polyacrylate. Interestingly, the electrochemical stability window of this electrolyte is extended greatly, even for high water contents. Particularly, the gel with 50?wt% ionomer exhibits an electrochemical stability window of 2.6?V vs. platinum and a conductivity of 6.5 mS cm-1 at 20?°C. Structural investigations suggest that the electrolytes locally self-organize and most likely switch local structures with the change of water content, leading to a 50% gel with good conductivity and elastic properties. A LiTi2(PO4)3/LiMn2O4 lithium-ion cell incorporating this electrolyte provided an average discharge voltage?>?1.5?V and a specific energy of 77?Wh?kg-1, while for an alternative cell chemistry, i.e., TiO2/LiMn2O4, a further enhanced average output voltage of 2.1?V and an initial specific energy of 124.2?Wh?kg-1 are achieved.

| S-EPMC6294254 | biostudies-other

Enhanced catalysis of radical-to-polysulfide interconversion <i>via</i> increased sulfur vacancies in lithium-sulfur batteries.

Project description:The practical application of lithium-sulfur (Li-S) batteries is seriously hindered by severe lithium polysulfide (LiPS) shuttling and sluggish electrochemical conversions. Herein, the Co9S8/MoS2 heterojunction as a model cathode host material is employed to discuss the performance improvement strategy and elucidate the catalytic mechanism. The introduction of sulfur vacancies can harmonize the chemisorption of the heterojunction component. Also, sulfur vacancies induce the generation of radicals, which participate in a liquidus disproportionated reaction to reduce the accumulation of liquid LiPSs. To assess the conversion efficiency from liquid LiPSs to solid Li2S, a new descriptor calculated from basic cyclic voltammetry curves, nucleation transformation ratio, is proposed.

| S-EPMC9159087 | biostudies-literature

The Polysulfide-Cathode Binding Energy Landscape for Lithium Sulfide Growth in Lithium-Sulfur Batteries.

Project description:A cathode substrate with strong adsorption of lithium polysulfides (LiPSs) has been preferred for lithium-sulfur (Li-S) batteries. However, the recent finding that controlled growth of lithium sulfides (Li2 S) during discharge is crucial for S utilization stimulates improvement of this preference. Here, the Li2 S growth and cell capacity in the LiPS binding energy landscape of cathode substrates are investigated. Specifically, Co-based ternary oxides are employed to obtain binding energies in the range of 4.0-7.4 eV. Of these substrates, only the MnCo2 O4 substrate with moderate LiPS affinity exhibits 3D Li2 S growth. The MnCo2 O4 cells achieve high sulfur utilization up to 84% at 0.2 C and excellent performance even under high sulfur loading/lean electrolyte conditions. In contrast, weak affinity substrates such as ZnCo2 O4 and strong affinity substrates such as NiCo2 O4 and CuCo2 O4 exhibit low discharge capacity with 2D Li2 S growth. For optimal LiPS affinity driving 3D growth, a balance between promoting LiPS adsorption and diffusion limitation in the LiPS adsorption layer is suggested.

| S-EPMC10131804 | biostudies-literature

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Project description:Bacterial cellulose nanofiber (BCNF) with high thermal stability produced by an ecofriendly process has emerged as a promising solution to realize safe and sustainable materials in the large-scale battery. However, an understanding of the actual thermal behavior of the BCNF in the full-cell battery has been lacking, and the yield is still limited for commercialization. Here, we report the entire process of BCNF production and battery manufacture. We systematically constructed a strain with the highest yield (31.5%) by increasing metabolic flux and improved safety by introducing a Lewis base to overcome thermochemical degradation in the battery. This report will open ways of exploiting the BCNF as a "single-layer" separator, a good alternative to the existing chemical-derived one, and thus can greatly contribute to solving the environmental and safety issues.

| S-EPMC6765254 | biostudies-literature

Influence of Lithium Polysulfide Clustering on the Kinetics of Electrochemical Conversion in Lithium-Sulfur Batteries.

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.

| S-EPMC7939025 | biostudies-literature

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