CO2 Laser Sintering of Garnet-Type Solid-State Electrolytes

Ramos, Erika; Browar, Allison; Roehling, John; Ye, Jianchao

doi:10.1021/acsenergylett.2c01630

CO₂ Laser Sintering of Garnet-Type Solid-State Electrolytes

Journal Article · Wed Sep 14 00:00:00 EDT 2022 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.2c01630· OSTI ID:1900323

Ramos, Erika ^[1]; Browar, Allison ^[1]; Roehling, John ^[1]; ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

We report the processing of garnet-type solid-state electrolytes remains challenging as densification conventionally requires high sintering temperatures and long processing times, which can result in severe Li loss, the formation of secondary phases, and thus high porosity and low ionic conductivity. Here, we report an ultrafast sintering method based on CO₂ laser scanning with the assistance of a heating stage. We demonstrate the rapid densification of low-packing-density Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) films, which are difficult to densify by conventional furnace sintering methods. This unique approach has three fingerprint characteristics: (1) mitigation of Li loss through ultrafast sintering (dwelling time $$\ll$$1 s); (2) a unique anisotropic shrinkage behavior that greatly reduces film thickness; (3) wave-like surface topology from point scanning strategy that enables 3D interfacial contacts with electrode materials. Herein, highly dense (95.68%) and highly conductive (0.26 mS·cm^–1 at 25 °C) LLZTO films are obtained through CO2 laser sintering. This work provides a unique, scalable, and widely applicable ultrarapid laser sintering technique to overcome the difficulties associated with classic methods for the integration of SSEs for practical all-solid-state Li-metal battery applications.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1900323

Report Number(s):: LLNL-JRNL-834792; 1053345

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 10 Vol. 7; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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