A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries

Luo, Chao; Hu, Enyuan; Gaskell, Karen J.; Fan, Xiulin; Gao, Tao; Cui, Chunyu; Ghose, Sanjit; Yang, Xiao-Qing; Wang, Chunsheng

doi:10.1073/pnas.2006301117

Title: A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries

Journal Article · Wed Jun 17 00:00:00 EDT 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.2006301117· OSTI ID:1633811

; Hu, Enyuan; Gaskell, Karen J.;

; Gao, Tao; Cui, Chunyu;

;

; Wang, Chunsheng

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: EE0008202; SC0012704; EE0008200

OSTI ID:: 1633811

Alternate ID(s):: OSTI ID: 1635484

Report Number(s):: BNL-216072-2020-JAAM

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 117 Journal Issue: 26; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 82 works

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lithium sulfur batteries
lean electrolyte
chemical bonding
carbon
oxygen

Title: A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries

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