Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 3, Pages 4051-4060Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c20139
Keywords
energy storage; solid-state batteries; solid-state electrolyte; electrochemistry; interfaces; lithium metal anode
Funding
- NASA Space Technology Research Fellowship
- Sloan Research Fellowship in Chemistry from the Alfred P. Sloan Foundation
- Ministry of Trade, Industry & Energy/Korea Institute of Energy Technology Evaluation and Planning (MOTIE/KETEP) [20194010000100]
- National Science Foundation [ECCS-2025462]
- Korea Evaluation Institute of Industrial Technology (KEIT) [20194010000100] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Solid-state batteries with lithium metal anodes offer higher specific energy, but require higher areal capacities and current densities for commercial viability. Research has focused on improving the rate capabilities of these batteries, with less attention paid to the impact of areal capacity on lithium plating/stripping behavior. This study investigates the relationship between areal capacity, current density, and plating/stripping stability, and quantifies the threshold capacity values for short circuiting.
Solid-state batteries (SSBs) with lithium metal anodes offer higher specific energy than conventional lithium-ion batteries, but they must utilize areal capacities >3 mAh cm(-2) and cycle at current densities >3 mA cm(-2) to achieve commercial viability. Substantial research effort has focused on increasing the rate capabilities of SSBs by mitigating detrimental processes such as lithium filament penetration and short circuiting. Less attention has been paid to understanding how areal capacity impacts lithium plating/stripping behavior in SSBs, despite the importance of areal capacity for achieving high specific energy. Here, we investigate and quantify the relationships among areal capacity, current density, and plating/stripping stability using both symmetric and full-cell configurations with a sulfide solid-state electrolyte (Li6PS5Cl). We show that unstable deposition and short circuiting readily occur at rates much lower than the measured critical current density when a sufficient areal capacity is passed. A systematic study of continuous plating under different electrochemical conditions reveals average threshold capacity values at different current densities, beyond which short circuiting occurs. Cycling cells below this threshold capacity significantly enhances cell lifetime, enabling stable symmetric cell cycling at 2.2 mA cm(-2) without short circuiting. Finally, we show that full cells with LiNi0.8Mn0.1Co0.1O2 also exhibit threshold capacity behavior, but they tend to short circuit at lower current densities and areal capacities. Our results quantify the effects of transferred capacity and demonstrate the importance of using realistic areal capacities in experiments to develop viable solid-state batteries.
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