Exploring the relationship between solvent-assisted ball milling, particle size, and sintering temperature in garnet-type solid electrolytes

Wood, Marissa; Gao, Xiaosi; Shi, Rongpei; Heo, Tae Wook; Espitia, Jose Ali; Duoss, Eric B.; Wood, Brandon C.; Ye, Jianchao

doi:10.1016/j.jpowsour.2020.229252

Exploring the relationship between solvent-assisted ball milling, particle size, and sintering temperature in garnet-type solid electrolytes

Journal Article · Tue Dec 08 00:00:00 EST 2020 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2020.229252· OSTI ID:1769095

Wood, Marissa ^[1]; Gao, Xiaosi ^[2]; ^[1]; ^[1]; ^[3]; ^[1]; ^[1]; ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Cornell Univ., Ithaca, NY (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of Texas, El Paso, TX (United States)

Garnet-type solid electrolytes, such as Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO), are promising materials for solid-state batteries, but processing remains a challenge, in part due to the high sintering temperature required for densification. Additionally, this temperature can be lowered by decreasing the initial particle size via solvent-assisted ball milling, but the relationship between solvent choice, particle properties, sintering behavior, and ionic conductivity is not well understood. In this work, we systematically explore these parameters, showing that milling in commonly used protic solvents, such as alcohols, effectively decreases the particle size but results in lithium loss (through Li⁺/H⁺ exchange) that leads to poor sintering. By contrast, milling in aprotic solvents with surfactant reduces the particle size to ~220 nm without lithium loss, enabling the fabrication of dense samples (5.1 g/cm³) with good ionic conductivity (0.43 mS/cm at 25 °C) at a lower sintering temperature (1000 °C). We compare ionic conductivities and activation energies for samples prepared with different particle sizes and sintering temperatures and use multiphase-field simulations to identify the mass transport and microstructural mechanisms responsible for the observed sintering dependence on particle size. These results further clarify the relationship between processing parameters and performance and represent important progress toward overcoming fabrication challenges for these materials.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1769095

Alternate ID(s):: OSTI ID: 1809615

Report Number(s):: LLNL-JRNL--811534; 1017493

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Journal Issue: na Vol. 484; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Exploring the relationship between solvent-assisted ball milling, particle size, and sintering temperature in garnet-type solid electrolytes

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