Title: Fluoro‐Ethylene‐Carbonate Plays a Double‐Edged Role on the Stability of Si Anode‐Based Rechargeable Batteries During Cycling and Calendar Aging

Journal Article · · Advanced Materials
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  1. Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99352 USA
  2. Energy and Environment Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
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Abstract The energy storage density of Li‐ion batteries can be improved by replacing graphite anodes with high‐capacity Si‐based materials, though instabilities have limited their implementation. Performance degradation mechanisms that occur in Si anodes can be divided into cycling stability (capacity retention after repeated battery cycles) and calendar aging (shelf life). While cycling instabilities and improvement strategies have been researched intensively, there is little known about the underlying mechanisms that cause calendar aging. In this work, multiple electron microscope techniques are used to explore the mechanism that governs calendar aging from the sub‐nanometer‐to‐electrode scale. Plasma focused ion beam tomography is used to create 3D reconstructions of calendar aged electrodes and revealed the growth of a LiF‐rich layer at the interface between the copper current collector and the silicon material, which can lead to delamination and increased interfacial impendence. The LiF layer appeared to derive from the fluoro‐ethylene‐carbonate electrolyte additive, which is commonly used to improve cycling stability in Si‐based systems. The results reveal that additives necessary to improve cycling stability can cause performance degradation over the long‐term during calendar aging. The results show that high performing, stable systems require careful design to simultaneously mitigate both cycling and calendar aging instabilities.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
2356855
Report Number(s):
PNNL-SA-195186; 2402625
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 30 Vol. 36; ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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25 ENERGY STORAGE
Si anode
battery
calendar life
cycle life