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Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion

Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion “Anode‐free” solid‐state batteries (SSBs), which have no anode active material, can exhibit extremely high energy density (≈1500 Wh L−1). However, there is a lack of understanding of the lithium plating/stripping mechanisms at initially lithium‐free solid‐state electrolyte (SSE) interfaces because excess lithium metal is often used. Here, it is demonstrated that commercially relevant quantities of lithium (>5 mAh cm−2) can be reliably plated at moderate current densities (1 mA cm−2) using the sulfide SSE Li6PS5Cl. Investigations of lithium plating/stripping mechanisms, in conjunction with cryo‐focused ion beam (FIB) imaging, synchrotron tomography, and phase‐field modeling, reveal that the cycling stability of these cells is fundamentally limited by the nonuniform presence of lithium during stripping. Local lithium depletion causes isolated lithium regions toward the end of stripping, decreasing electrochemically active area and resulting in high local current densities and void formation. This accelerates subsequent filament growth and short circuiting compared to lithium‐excess cells. Despite this degradation mode, it is shown that anode‐free cells exhibit comparable Coulombic efficiency to lithium‐excess cells, and improved resistance to short circuiting is achieved by avoiding local lithium depletion through retention of thicker lithium at the interface. These new insights provide a foundation for engineering future high‐energy anode‐free SSBs. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Energy Materials Wiley

Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion

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References (41)

Publisher
Wiley
Copyright
© 2023 Wiley‐VCH GmbH
ISSN
1614-6832
eISSN
1614-6840
DOI
10.1002/aenm.202204186
Publisher site
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Abstract

“Anode‐free” solid‐state batteries (SSBs), which have no anode active material, can exhibit extremely high energy density (≈1500 Wh L−1). However, there is a lack of understanding of the lithium plating/stripping mechanisms at initially lithium‐free solid‐state electrolyte (SSE) interfaces because excess lithium metal is often used. Here, it is demonstrated that commercially relevant quantities of lithium (>5 mAh cm−2) can be reliably plated at moderate current densities (1 mA cm−2) using the sulfide SSE Li6PS5Cl. Investigations of lithium plating/stripping mechanisms, in conjunction with cryo‐focused ion beam (FIB) imaging, synchrotron tomography, and phase‐field modeling, reveal that the cycling stability of these cells is fundamentally limited by the nonuniform presence of lithium during stripping. Local lithium depletion causes isolated lithium regions toward the end of stripping, decreasing electrochemically active area and resulting in high local current densities and void formation. This accelerates subsequent filament growth and short circuiting compared to lithium‐excess cells. Despite this degradation mode, it is shown that anode‐free cells exhibit comparable Coulombic efficiency to lithium‐excess cells, and improved resistance to short circuiting is achieved by avoiding local lithium depletion through retention of thicker lithium at the interface. These new insights provide a foundation for engineering future high‐energy anode‐free SSBs.

Journal

Advanced Energy Materials – Wiley

Published: Mar 1, 2023

Keywords: electrochemistry; energy storage; lithium metal anodes; solid‐state batteries; X‐ray tomography

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