Li-Sb Alloy Formation Strategy to Improve Interfacial Stability of All-Solid-State Lithium Batteries

Berhanu Degagsa Dandena; Wei-Nien Su; Dah-Shyang Tsai; Yosef Nikodimos; Bereket Woldegbreal Taklu; Hailemariam Kassa Bezabh; Gidey Bahre Desta; Sheng-Chiang Yang; Keseven Lakshmanan; Hwo-Shuenn Sheu; Chia-Hsin Wang; She-Huang Wu; Bing Joe Hwang

doi:10.1002/smtd.202400571

Li-Sb Alloy Formation Strategy to Improve Interfacial Stability of All-Solid-State Lithium Batteries

Small Methods. 2024 Oct 4:e2400571. doi: 10.1002/smtd.202400571. Online ahead of print.

Authors

Berhanu Degagsa Dandena^{1

2}, Wei-Nien Su^{2

3}, Dah-Shyang Tsai¹, Yosef Nikodimos^{1

2}, Bereket Woldegbreal Taklu^{1

2}, Hailemariam Kassa Bezabh¹, Gidey Bahre Desta³, Sheng-Chiang Yang^{1

2}, Keseven Lakshmanan^{1

2}, Hwo-Shuenn Sheu⁴, Chia-Hsin Wang⁴, She-Huang Wu^{2

3}, Bing Joe Hwang^{1

2

4}

Affiliations

¹ Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei, 106, Taiwan.
² Sustainable Electrochemical Energy Development Center, National Taiwan University of Science and Technology, Taipei, 106, Taiwan.
³ Nano-electrochemistry Laboratory, Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei, 106, Taiwan.
⁴ National Synchrotron Radiation Research Center (NSRRC), Hsin-chu, 30076, Taiwan.

PMID: 39367548
DOI: 10.1002/smtd.202400571

Abstract

The solid electrolyte is anticipated to prevent lithium dendrite formation. However, preventing interface reactions and the development of undesirable lithium metal deposition during cycling are difficult and remain unresolved. Here, to comprehend these occurrences better, this study reports an alloy formation strategy for enhanced interface stability by incorporating antimony (Sb) in the lithium argyrodite solid electrolyte Li₆PS₅Cl (LPSC-P) to form Li-Sb alloy. The Li-Sb alloy emergence at the anodic interface is crucial in facilitating uniform lithium deposition, resulting in excellent long-term stability, and achieving the highest critical current density of 14.5 mA cm^-2 (among the reported sulfide solid electrolytes) without lithium dendrite penetration. Furthermore, Li-Sb alloy formation maintain interfacial contact, even, after several plating and stripping. The Li-Sb alloy formation is confirmed by XRD, Raman, and XPS. The work demonstrates the prospect of utilizing alloy-forming electrolytes for advanced solid-state batteries.

Keywords: H2S; Li‐argyrodite solid electrolyte; Sb‐doped; alloy formation; interface stability.

Abstract

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