Rapid Laser Reactive Sintering of Garnet Li6.4La3Zr1.4Ta0.6O12 and Li6.1La3Zr2Al0.3O12 and Solid-State Electrolytes
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
All solid-state lithium-ion batteries (ASSLIBs) have gained significant interest in recent years due to their wide range of applications, including mobile devices, electric vehicles, and grid storage. Garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte (SSE) continues to be a significant player in the fabrication of ASSLIBs with excellent ionic conductivity on the order of 10-3 S•cm-1 with the integration of dopants and sintering aids to assist conductivity and structural evolution during the sintering procedure. Traditional sintering techniques, such as solid-state sintering (SSS), have been proven to yield desirable crystal structures. However, the low ionic conductivity results from inferior microstructure, and lithium loss is a significant challenge. Recently, a relatively novel sintering process called rapid laser sintering (RLS) has shown great potential for achieving fully dense solid oxide electrolytes with less lithium loss, resulting in high ionic conductivity [1] [2] [3] [4]. Here, we applied a modified RLS method using precursor powders instead of pre-synthesized LLZO powders to fabricate Al-doped LLZO (Li6.1La3Zr2Al0.3O12 + 13 wt% Li2CO3) and Ta-doped LLZO (Li6.4La3Zr1.4Ta0.6O12 + 5 wt% LiOH•H2O) dense electrolytes. This rapid laser reactive sintering (RLRS) could potentially reduce the number of processing steps and therefore lower the manufacturing cost. We hope the rapid high-temperature sintering can densify the electrolyte and avoid the lithium loss for achieving high lithium-ion conductivity. In this work, we optimized a combination of laser parameters (speed and power), initial precursor composition, and controlled atmospheres to discover the optimal conditions for reaching the efficacious crystal structure, microstructure, and ionic conductivity.
- Research Organization:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Organization:
- USDOE National Nuclear Security Administration (NNSA)
- DOE Contract Number:
- AC52-07NA27344
- OSTI ID:
- 2205719
- Report Number(s):
- LLNL-TR-854301; 1082683
- Country of Publication:
- United States
- Language:
- English
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