A Fluorinated Lewis Acidic Organoboron Tunes Polysulfide Complex Structure for High–Performance Lithium–Sulfur Batteries

Gao, Siyuan; Li, Bomin; Zhu, Qijia; Yang, Jingtian; Xu, Jiayi; An, Bowen; Liu, Cong; Wu, Qin; Liu, Qian; Zhang, Zhengcheng; Cheng, Yingwen

doi:10.1002/aenm.202403439

Title: A Fluorinated Lewis Acidic Organoboron Tunes Polysulfide Complex Structure for High–Performance Lithium–Sulfur Batteries

Journal Article · 16 September 2024 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202403439 · OSTI ID:2448267

Gao, Siyuan ^[1]; Li, Bomin ^[2]; Zhu, Qijia ^[3]; Yang, Jingtian ^[3]; Xu, Jiayi ^[3]; An, Bowen ^[2]; Liu, Cong ^[3];

^[4]; Liu, Qian ^[3]; Zhang, Zhengcheng ^[3];

^[1]

Univ. of Tennessee, Knoxville, TN (United States); Northern Illinois Univ., DeKalb, IL (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Many challenges in lithium-sulfur (Li–S) batteries are associated with the radical change in lithium polysulfide (LPS) solubility during cycling, but chemical approaches to address such inconsistency are still lacking. Here, the use of a strong Lewis acidic fluorinated organoboron, tri(2,2,2-trifluoroethyl) borate (TFEB), is reported as a multi-functional mediator to simultaneously overcome multiple technical barriers in practical Li–S batteries. TFEB acts as an anion acceptor and forms strong molecular complexes with Lewis basic LPS. The TFEB-LPS complexes have consistent solubility across the full polysulfide spectrum and deliver several times improved better redox kinetics, unlocking a true redox catalytic mechanism that covers the majority of redox events in thick sulfur cathodes. As a result, Li–S batteries evaluated under practical conditions exhibit significantly improved discharge capacity, rate capability, and cycling stability with the addition of the TFEB additive. More importantly, TFEB also contributes to the stabilization of lithium anode in the presence of polysulfides by generating strong interfacial film. These attributes significantly improve the cycling stability of practical Li–S pouch cells, which are assembled with a unit energy density of 219 Wh kg^–1. Finally, the results provide new molecular insights on the design of unlocking solvation networks of practical Li–S systems.

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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:: 2448267

Report Number(s):: BNL--226144-2024-JAAM

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 6 Vol. 15; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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lithium-sulfur battery
multi-functional mediator
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2-trifluoroethyl) borate

Title: A Fluorinated Lewis Acidic Organoboron Tunes Polysulfide Complex Structure for High–Performance Lithium–Sulfur Batteries

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