Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 28, Pages 15503-15509Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103470
Keywords
electrolyte structure; lithium metal anode; lithium-sulfur batteries; polysulfide encapsulation; solvent shell
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Funding
- National Natural Science Foundation of China [U1801257, 22061132002, 21825501]
- National Key Research and Development Program [2016YFA0202500]
- Natural Sciences and Engineering Research Council of Canada [NSERC RGPIN-2017-05080]
- Westgrid
- Canada First Research Excellence Fund
- Compute Canada
- Tsinghua University Initiative Scientific Research Program
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This study reveals the electrolyte structure of PSs with anti-reductive solvent shells, reducing the reactivity between PSs and Li and significantly improving the cycling performance of Li-S batteries.
The lithium-sulfur (Li-S) battery is regarded as a promising secondary battery. However, constant parasitic reactions between the Li anode and soluble polysulfide (PS) intermediates significantly deteriorate the working Li anode. The rational design to inhibit the parasitic reactions is plagued by the inability to understand and regulate the electrolyte structure of PSs. Herein, the electrolyte structure of PSs with anti-reductive solvent shells was unveiled by molecular dynamics simulations and nuclear magnetic resonance. The reduction resistance of the solvent shell is proven to be a key reason for the decreased reactivity of PSs towards Li. With isopropyl ether (DIPE) as a cosolvent, DIPE molecules tend to distribute in the outer solvent shell due to poor solvating power. Furthermore, DIPE is more stable than conventional ether solvents against Li metal. The reactivity of PSs is suppressed by encapsulating PSs into anti-reductive solvent shells. Consequently, the cycling performance of working Li-S batteries was significantly improved and a pouch cell of 300 Wh kg(-1) was demonstrated. The fundamental understanding in this work provides an unprecedented ground to understand the electrolyte structure of PSs and the rational electrolyte design in Li-S batteries.
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