High Energy Density Lithium–Sulfur Batteries Based on Carbonaceous Two-Dimensional Additive Cathodes
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PROVIDER: S-EPMC10052352 | biostudies-literature | 2023 Mar
REPOSITORIES: biostudies-literature
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Project description:How to exert the energy density advantage is a key link in the development of lithium-sulfur batteries. Therefore, the performance degradation of high-sulfur-loading cathodes becomes an urgent problem to be solved at present. In addition, the volumetric capacities of high-sulfur-loading cathodes are still at a low level compared with their areal capacities. Aiming at these issues, two-dimensional carbon yolk-shell nanosheet is developed herein to construct a novel self-supporting sulfur cathode. The cathode with high-sulfur loading of 5 mg cm-2 and sulfur content of 73 wt% not only delivers an excellent rate performance and cycling stability, but also provides a favorable balance between the areal (5.7 mAh cm-2) and volumetric (1330 mAh cm-3) capacities. Remarkably, an areal capacity of 11.4 mAh cm-2 can be further achieved by increasing the sulfur loading from 5 to 10 mg cm-2. This work provides a promising direction for high-energy-density lithium-sulfur batteries.One of the challenges facing lithium-sulfur batteries is to develop cathodes with high mass and high volume loading. Here the authors show that two-dimensional carbon yolk-shell nanosheets are promising sulfur host materials, enabling stable battery cells with high energy density.
| S-EPMC5589916 | biostudies-literature
Project description:Rechargeable lithium-sulfur (Li-S) batteries are receiving ever-increasing attention due to their high theoretical energy density and inexpensive raw sulfur materials. However, their rapid capacity fade has been one of the key barriers for their further improvement. It is well accepted that the major degradation mechanisms of S-cathodes include low electrical conductivity of S and sulfides, precipitation of nonconductive Li2S2 and Li2S, and poly-shuttle effects. To determine these degradation factors, a comprehensive study of sulfur cathodes with different amounts of electrolytes is presented here. A survey of the fundamentals of Li-S chemistry with respect to capacity fade is first conducted; then, the parameters obtained through electrochemical performance and characterization are used to determine the key causes of capacity fade in Li-S batteries. It is confirmed that the formation and accumulation of nonconductive Li2S2/Li2S films on sulfur cathode surfaces are the major parameters contributing to the rapid capacity fade of Li-S batteries.
| S-EPMC5157169 | biostudies-literature
Project description:Owing to the overwhelming advantage in energy density, lithium-sulfur (Li-S) battery is a promising next-generation electrochemical energy storage system. Despite many efforts in pursuing long cycle life, relatively little emphasis has been placed on increasing the areal energy density. Herein, we have designed and developed a 'pie' structured electrode, which provides an excellent balance between gravimetric and areal energy densities. Combining lotus root-like multichannel carbon nanofibers 'filling' and amino-functionalized graphene 'crust', the free-standing paper electrode (S mass loading: 3.6 mg cm(-2)) delivers high specific capacity of 1,314 mAh g(-1) (4.7 mAh cm(-2)) at 0.1 C (0.6 mA cm(-2)) accompanied with good cycling stability. Moreover, the areal capacity can be further boosted to more than 8 mAh cm(-2) by stacking three layers of paper electrodes with S mass loading of 10.8 mg cm(-2).
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Project description:Trapping lithium polysulfides (LiPSs) on a material effectively suppresses the shuttle effect and enhances the cycling stability of Li-S batteries. For the first time, we advocate a recently synthesized two-dimensional material, biphenylene, as an anchoring material for the lithium-sulfur battery. The density functional theory calculations show that LiPSs bind with pristine biphenylene insubstantially with binding energy ranging from -0.21 eV to -1.22 eV. However, defect engineering through a single C atom vacancy significantly improves the binding strength (binding energy in the range -1.07 to -4.11 eV). The Bader analysis reveals that LiPSs and S8 clusters donate the charge (ranging from -0.05 e to -1.12 e) to the biphenylene sheet. The binding energy of LiPSs with electrolytes is smaller than those with the defective biphenylene sheet, which provides its potential as an anchoring material. Compared with other reported two-dimensional materials such as graphene, MXenes, and phosphorene, the biphenylene sheet exhibits higher binding energies with the polysulfides. Our study deepens the fundamental understanding and shows that the biphenylene sheet is an excellent anchoring material for lithium-sulfur batteries for suppressing the shuttle effect because of its superior conductivity, porosity, and strong anchoring ability.
| S-EPMC8931010 | biostudies-literature
Project description:An upgrade of the scalable fabrication of high-performance sulfur-carbon cathodes is essential for the widespread commercialization of this technology. Herein we present a simple, cost-effective and scalable approach for the fabrication of cathodes comprising sulfur and high-surface area, N,S-codoped carbons. The method involves the use of a sulfur salt, i.e. sodium thiosulfate, as activating agent, sulfur precursor and S-dopant, and polypyrrole as carbon precursor and N-dopant. In this way, the production of the porous host and the incorporation of sulfur are combined in the same procedure. The porous hosts thus produced have BET surface areas in excess of 2000 m2 g-1, a micro-mesoporous structure, as well as sulfur and nitrogen contents of 5-6 wt% and ~2 wt%, respectively. The elemental sulfur content in the composites can be precisely modulated in the range of 24 to ca. 90 wt% by controlling the amount of sodium thiosulfate used. Remarkably, these porous carbons are able to accommodate up to 80 wt% sulfur exclusively within their porosity. When analyzed in lithium-sulfur batteries, these sulfur-carbon composites show high specific capacities of 1100 mAh g-1 at a low C-rate of 0.1 C and above 500 mAh g-1 at a high rate of 2 C for sulfur contents in the range of 50-80 wt%. Remarkably, the composites with 51-65 wt% S can still provide above 400 mAh g-1 at an ultra-fast rate of 4 C (where a charge and discharge cycle takes only ten minutes). The good rate capability and sulfur utilization was additionally assessed for cathodes with a high sulfur content (65-74%) and a high sulfur loading (>5 mg cm-2). In addition, cathodes of 4 mg cm-2 successfully cycled for 260 cycles at 0.2 C showed only a low loss of 0.12%/cycle.
| S-EPMC7078249 | biostudies-literature
Project description:Herein, the concept of constructing binder- and carbon additive-free organosulfur cathode was proved based on thiol-containing conducting polymer poly(4-(thiophene-3-yl) benzenethiol) (PTBT). The PTBT featured the polythiophene-structure main chain as a highly conducting framework and the benzenethiol side chain to copolymerize with sulfur and form a crosslinked organosulfur polymer (namely S/PTBT). Meanwhile, it could be in-situ deposited on the current collector by electro-polymerization, making it a binder-free and free-standing cathode for Li-S batteries. The S/PTBT cathode exhibited a reversible capacity of around 870 mAh g-1 at 0.1 C and improved cycling performance compared to the physically mixed cathode (namely S&PTBT). This multifunction cathode eliminated the influence of the additives (carbon/binder), making it suitable to be applied as a model electrode for operando analysis. Operando X-ray imaging revealed the remarkable effect in the suppression of polysulfides shuttle via introducing covalent bonds, paving the way for the study of the intrinsic mechanisms in Li-S batteries.
| S-EPMC9401019 | biostudies-literature
Project description:Lithium-sulfur batteries can displace lithium-ion by delivering higher specific energy. Presently, however, the superior energy performance fades rapidly when the sulfur electrode is loaded to the required levels-5 to 10 mg cm-2- due to substantial volume change of lithiation/delithiation and the resultant stresses. Inspired by the classical approaches in particle agglomeration theories, we found an approach that places minimum amounts of a high-modulus binder between neighboring particles, leaving increased space for material expansion and ion diffusion. These expansion-tolerant electrodes with loadings up to 15 mg cm-2 yield high gravimetric (>1200 mA·hour g-1) and areal (19 mA·hour cm-2) capacities. The cells are stable for more than 200 cycles, unprecedented in such thick cathodes, with Coulombic efficiency above 99%.
| S-EPMC6941919 | biostudies-literature
Project description:The lithium-sulfur battery has long been seen as a potential next generation battery chemistry for electric vehicles owing to the high theoretical specific energy and low cost of sulfur. However, even state-of-the-art lithium-sulfur batteries suffer from short lifetimes due to the migration of highly soluble polysulfide intermediates and exhibit less than desired energy density due to the required excess electrolyte. The use of sparingly solvating electrolytes in lithium-sulfur batteries is a promising approach to decouple electrolyte quantity from reaction mechanism, thus creating a pathway toward high energy density that deviates from the current catholyte approach. Herein, we demonstrate that sparingly solvating electrolytes based on compact, polar molecules with a 2:1 ratio of a functional group to lithium salt can fundamentally redirect the lithium-sulfur reaction pathway by inhibiting the traditional mechanism that is based on fully solvated intermediates. In contrast to the standard catholyte sulfur electrochemistry, sparingly solvating electrolytes promote intermediate- and short-chain polysulfide formation during the first third of discharge, before disproportionation results in crystalline lithium sulfide and a restricted fraction of soluble polysulfides which are further reduced during the remaining discharge. Moreover, operation at intermediate temperatures ca. 50 °C allows for minimal overpotentials and high utilization of sulfur at practical rates. This discovery opens the door to a new wave of scientific inquiry based on modifying the electrolyte local structure to tune and control the reaction pathway of many precipitation-dissolution chemistries, lithium-sulfur and beyond.
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Project description:It is a great challenge to obtain high performance carbon fluoride (CF x ) cathodes with high specific capacity and good rate performance due to the electronic conductivity of CF x being known to decrease with an increase in the specific capacity. Herein, we propose a novel fluorinated graphene (FG)/sulfur hybrid cathode to enhance both the energy density and power density of lithium/carbon fluoride (Li/CF x ) batteries. Impressive enhancements of the specific capacity, discharge voltage, and rate capability are demonstrated with the novel FG/sulfur hybrid cathode. In comparison with the pristine FG cathode, the hybrid cathode exhibits higher electrochemical activity, lower overpotential, and faster ion transfer over the main discharge range. Furthermore, when the melt-diffusion method is used to prepare the hybrid cathode, the uncommon monoclinic sulfur is presented under ambient temperature. A significant synergistic effect which reduces the reaction resistance effectively is demonstrated with the presence of monoclinic sulfur, leading to the highest energy density of 2341 W h kg-1 and a power density up to 13 621 W kg-1 at 8.0 A g-1. Our results are expected to introduce a new generation of high energy and high power density lithium primary cells, based on a simple and effective strategy employing FG/S hybrid cathodes.
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Project description: Not available
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