Custom-form iron trifluoride Li-batteries using material extrusion and electrolyte exchanged ionogels

Journal Article · 27 March 2024 · Additive Manufacturing

DOI: https://doi.org/10.1016/j.addma.2024.104102 · OSTI ID:2371081

Cardenas, Jorge Antonio ^[1]; Bullivant, John Paul ^[1]; Wygant, Bryan Russell ^[1]; Lapp, Aliya Siegel ^[2]; Bell, Nelson S. ^[1]; Lambert, Timothy N. ^[1]; Merrill, Laura Christine ^[1]; Talin, Albert Alec ^[2]; Cook, Adam W. ^[1]; Allcorn, Eric Koederitz ^[1]; Harrison, Katharine Lee ^[3]

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1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
2. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Custom-form factor batteries fabricated in non-conventional shapes can maximize the overall energy density of the systems they power, particularly when used in conjunction with energy dense materials (e.g., Li metal anodes and conversion cathodes). Additive manufacturing (AM), and specifically material extrusion (ME), have been shown as effective methods for producing custom-form cell components, particularly electrodes. However, the AM of several promising energy dense materials (conversion electrodes such as iron trifluoride) have yet to be demonstrated or optimized. Furthermore, the integration of multiple AM produced cell components, such as electrodes and separators, along with a custom package remains largely unexplored. In this work, iron trifluoride (FeF₃) and ionogel (IG) separators are conformally printed using ME onto non-planar surfaces to enable the fabrication of custom-form Li-FeF₃ batteries. Further, to demonstrate printing on non-planar surfaces, cathodes and separators were deposited onto cylindrical rods using a 5-axis ME printer. ME printed FeF₃ was shown to have performance commensurate with FeF₃ cast using conventional means, both in coin cell and cylindrical rod formats, with capacities exceeding 700 mAh/g on the first cycle and ranging between 600 and 400 mAh/g over the next 50 cycles. Additionally, a ME process for printing polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) based IGs directly onto FeF₃ is developed and enabled using an electrolyte exchange process. In coin cells, this process is shown to produce cells with similar capacity to cells built with Celgard separators out to 50 cycles, with the exception that cycling instabilities are observed during cycles 8–20. When using printed and exchanged IGs in a custom cylindrical cell package, 6 stable high-capacity cycles are achieved. Overall, this work demonstrates approaches for producing high-energy-density Li-FeF₃ cells in coin and cylindrical rod formats, which are translatable to customized, arbitrary geometries compatible with ME printing and electrolyte exchange.

• Research Organization: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
• Grant/Contract Number: NA0003525; AC36-08GO28308
• OSTI ID: 2371081
• Alternate ID(s): OSTI ID: 2333055
• Report Number(s): SAND--2024-07158J
• Journal Information: Additive Manufacturing, Journal Name: Additive Manufacturing Vol. 84; ISSN 2214-8604
• Publisher: ElsevierCopyright Statement
• Country of Publication: United States
• Language: English