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A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries.

ABSTRACT: Lithium sulfur batteries (LSBs) are promising next-generation rechargeable batteries due to the high gravimetric energy, low cost, abundance, nontoxicity, and high sustainability of sulfur. However, the dissolution of high-order polysulfide in electrolytes and low Coulombic efficiency of Li anode require excess electrolytes and Li metal, which significantly reduce the energy density of LSBs. Quasi-solid-state LSBs, where sulfur is encapsulated in the micropores of carbon matrix and sealed by solid electrolyte interphase, can operate under lean electrolyte conditions, but a low sulfur loading in carbon matrix (<40 wt %) and low sulfur unitization (<70%) still limit the energy density in a cell level. Here, we significantly increase the sulfur loading in carbon to 60 wt % and sulfur utilization to ?87% by dispersing sulfur in an oxygen-rich dense carbon host at a molecular level through strong chemical interactions of C-S and O-S. In an all-fluorinated organic lean electrolyte, the C/S cathode experiences a solid-state lithiation/delithiation reaction after the formation of solid electrolyte interphase in the first deep lithiation, completely avoiding the shuttle reaction. The chemically stabilized C/S composite retains a high reversible capacity of 541 mAh?g-1 (based on the total weight of the C/S composite) for 200 cycles under lean electrolyte conditions, corresponding to a high energy density of 974 Wh?kg-1 The superior electrochemical performance of the chemical bonding-stabilized C/S composite renders it a promising cathode material for high-energy and long-cycle-life LSBs.

SUBMITTER: Luo C

PROVIDER: S-EPMC7334495 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries.

Luo Chao C Hu Enyuan E Gaskell Karen J KJ Fan Xiulin X Gao Tao T Cui Chunyu C Ghose Sanjit S Yang Xiao-Qing XQ Wang Chunsheng C

Proceedings of the National Academy of Sciences of the United States of America 20200617 26

Lithium sulfur batteries (LSBs) are promising next-generation rechargeable batteries due to the high gravimetric energy, low cost, abundance, nontoxicity, and high sustainability of sulfur. However, the dissolution of high-order polysulfide in electrolytes and low Coulombic efficiency of Li anode require excess electrolytes and Li metal, which significantly reduce the energy density of LSBs. Quasi-solid-state LSBs, where sulfur is encapsulated in the micropores of carbon matrix and sealed by sol ...[more]

PMID: 32554498

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Project description:With the development of mobile electronic devices, there are more and more requirements for high-energy storage equipment. Traditional lithium-ion batteries, like lithium-iron phosphate batteries, are limited by their theoretical specific capacities and might not meet the requirements for high energy density in the future. Lithium-sulfur batteries (LSBs) might be ideal next-generation energy storage devices because they have nearly 10 times the theoretical specific capacities of lithium-ion batteries. However, the severe capacity decay of LSBs limits their application, especially at high currents. In this study, an ionic liquid (IL) electrolyte additive, TDA+TFSI, was reported. When 5% of the TDA+TFSI additive was added to a traditional ether-based organic electrolyte, the cycling performance of the LSBs was significantly improved compared with that of the LSBs with the pure traditional organic electrolyte. At a rate of 0.5 C, the discharge specific capacity in the first cycle of the LSBs with the 5% TDA+TFSI electrolyte additive was 1167 mAh g-1; the residual specific capacities after 100 cycles and 300 cycles were 579 mAh g-1 and 523 mAh g-1, respectively; and the average capacity decay rate per cycle was only 0.18% in 300 cycles. Moreover, the electrolyte with the TDA+TFSI additive had more obvious advantages than the pure organic ether-based electrolyte at high charge and discharge currents of 1.0 C. The residual discharge specific capacities were 428 mAh g-1 after 100 cycles and 399 mAh g-1 after 250 cycles, which were 13% higher than those of the LSBs without the TDA+TFSI additive. At the same time, the Coulombic efficiencies of the LSBs using the TDA+TFSI electrolyte additive were more stable than those of the LSBs using the traditional organic ether-based electrolyte. The results showed that the LSBs with the TDA+TFSI electrolyte additive formed a denser and more uniform solid electrolyte interface (SEI) film during cycling, which improved the stability of the electrochemical reaction.

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A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries.

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A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries.

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