High Sulfur Loading and Capacity Retention in Bilayer Garnet Sulfurized‐Polyacrylonitrile/Lithium‐Metal Batteries with Gel Polymer Electrolytes

Shi, Changmin; Takeuchi, Saya; Alexander, George V.; Hamann, Tanner; O'Neill, Jonathan; Dura, Joseph A.; Wachsman, Eric D.

doi:10.1002/aenm.202301656

High Sulfur Loading and Capacity Retention in Bilayer Garnet Sulfurized‐Polyacrylonitrile/Lithium‐Metal Batteries with Gel Polymer Electrolytes (in EN)

Journal Article · Sun Sep 24 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202301656· OSTI ID:2575801

^[1]; Takeuchi, Saya ^[2]; Alexander, George V. ^[1]; Hamann, Tanner ^[1]; O'Neill, Jonathan ^[1]; Dura, Joseph A. ^[3]; ^[1]

Univ. of Maryland, College Park, MD (United States)
Univ. of Maryland, College Park, MD (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)

The cubic‐garnet (Li₇La₃Zr₂O₁₂, LLZO) lithium–sulfur battery shows great promise in the pursuit of achieving high energy densities. The sulfur used in the cathodes is abundant, inexpensive, and possesses high specific capacity. In addition, LLZO displays excellent chemical stability with Li metal; however, the instabilities in the sulfur cathode/LLZO interface can lead to performance degradation that limits the development of these batteries. Therefore, it is critical to resolve these interfacial challenges to achieve stable cycling. Here, an innovative gel polymer buffer layer to stabilize the sulfur cathode/LLZO interface is created. Employing a thin bilayer LLZO (dense/porous) architecture as a solid electrolyte and significantly high sulfur loading of 5.2 mg cm⁻², stable cycling is achieved with a high initial discharge capacity of 1542 mAh g⁻¹ (discharge current density of 0.87 mA cm⁻²) and an average discharge capacity of 1218 mAh g⁻¹ (discharge current density of 1.74 mA cm⁻²) with 80% capacity retention over 265 cycles, at room temperature (22 °C) and without applied pressure. Achieving such stability with high sulfur loading is a major step in the development of potentially commercial garnet lithium–sulfur batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Maryland, College Park, MD (United States)

Sponsoring Organization:: US Army Research Laboratory; USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AR0000787

OSTI ID:: 2575801

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 42 Vol. 13; ISSN 1614-6840; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: EN

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