Anode-Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

Ren, Yuxun; Bhargav, Amruth; Shin, Woochul; Sul, Hyunki; Manthiram, Arumugam

doi:10.1002/anie.202207907

Anode-Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

Journal Article · Thu Jul 07 00:00:00 EDT 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202207907· OSTI ID:1976284

Ren, Yuxun ^[1]; Bhargav, Amruth ^[2]; Shin, Woochul ^[2]; Sul, Hyunki ^[2]; ^[2]

Univ. of Texas, Austin, TX (United States); OSTI
Univ. of Texas, Austin, TX (United States)

The two major barriers of practical lithium–sulfur batteries are the poor reversibility of lithium-metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. In this study, we show that SnI₄ coordinates with lithium polysulfides to form soluble complexes, resulting in a Li₂SnS₃-rich anode interphase layer. As Li₂SnS₃ is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI₄ and lithium polysulfides play a non-negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode-free, lean-electrolyte pouch cells with a Li₂S cathode that displays capacity retention of 78 % after 100 cycles.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States); University of Texas, Austin, TX (United States)

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

Grant/Contract Number:: EE0007762

OSTI ID:: 1976284

Alternate ID(s):: OSTI ID: 1882752
OSTI ID: 2217438

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 35 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Anode-Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

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