Addressing Passivation in Lithium-Sulfur Battery Under Lean Electrolyte Condition

Pan, Huilin; Han, Kee Sung; Engelhard, Mark H.; Cao, Ruiguo; Chen, Junzheng; Zhang, Ji-Guang; Mueller, Karl T.; Shao, Yuyan; Liu, Jun

doi:10.1002/adfm.201707234

Addressing Passivation in Lithium-Sulfur Battery Under Lean Electrolyte Condition

Journal Article · Thu Feb 22 23:00:00 EST 2018 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.201707234· OSTI ID:1490342

^[1]; Han, Kee Sung ^[2]; Engelhard, Mark H. ^[3]; Cao, Ruiguo ^[1]; Chen, Junzheng ^[1]; Zhang, Ji-Guang ^[1]; Mueller, Karl T. ^[4]; Shao, Yuyan ^[1]; Liu, Jun ^[1]

Joint Center for Energy Storage Research (JCESR), Pacific Northwest National Laboratory, Richland WA 99352 USA; Energy and Environmental Directorate, Pacific Northwest National Laboratory, Richland WA 99352 USA
Joint Center for Energy Storage Research (JCESR), Pacific Northwest National Laboratory, Richland WA 99352 USA; Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland WA 99352 USA
Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland WA 99352 USA
Joint Center for Energy Storage Research (JCESR), Pacific Northwest National Laboratory, Richland WA 99352 USA; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland WA 99352 USA

Reducing the electrolyte amount is critical for high practical specific energy of Li-S batteries. The lean electrolyte condition raises a complex situation for sulfur redox reactions since they rely on the electrolyte mediation. The insulating nature of discharge product Li₂S and its uncontrollable accumulation (passivation) at the cathode interface is one of the major challenges for stable cycling of a Li-S battery under lean electrolyte condition. Here, we present that the NH₄TFSI additive in electrolyte solution greatly alleviates the passivation issue in Li-S batteries under lean electrolyte condition. The ammonium additive enhances the solvation between sulfide anion and NH₄⁺ cation, and greatly reduces the amount of large insoluble and insulting Li₂S particles in the sulfur cathodes, which greatly facilitates the reversible and sustainable redox reactions of sulfur. Therefore, the cycle life of Li-S battery under lean electrolyte condition was greatly improved. In addition, we found that the morphology of Li anode is dependent on the cathode structures. Ammonium additive enables a homogeneous surface of cathode and Li anode and extended cycle life.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1490342

Report Number(s):: PNNL-SA-131237

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 38 Vol. 28; ISSN 1616-301X

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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