A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li–S Batteries

Qin, Kaiqiang; Li, Shi; Yen, Dean; Zhang, Weiran; Yang, Zhenzhen; Kamphaus, Ethan Phillip; Kim, Eric Youngsam; Huang, Jinghao; Shea, John J.; Hu, Enyuan; Cheng, Lei; Wang, Chunsheng; Luo, Chao

doi:10.1021/acsenergylett.4c00859

A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li–S Batteries

Journal Article · Mon Jul 15 00:00:00 EDT 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.4c00859· OSTI ID:2433978

Qin, Kaiqiang ^[1]; Li, Shi ^[2]; Yen, Dean ^[3]; Zhang, Weiran ^[4]; ^[2]; ^[2]; Kim, Eric Youngsam ^[1]; Huang, Jinghao ^[5]; Shea, John J. ^[1]; ^[3]; ^[6]; ^[4]; ^[5]

George Mason Univ., Fairfax, VA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Univ. of Maryland, College Park, MD (United States)
George Mason Univ., Fairfax, VA (United States); Univ. of Miami, Coral Gables, FL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte condition. Herein, a LiF-rich SEI and a LiF-Li_xN_yO_z co-enriched CEI are simultaneously formed by adding ionic liquid (Py₁₃TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. In this study, the LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN and therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm^-2) pouch cells under the lean electrolyte condition (E/S ratio of 5 mL g_SPAN^-1) delivers a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium-sulfur batteries.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2433978

Report Number(s):: BNL--225982-2024-JAAM

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 8 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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