Appendix G: Rapid Laser Reactive Sintering of High-Performance Electrolytes for Additive Manufacturing of Solid State Batteries

State-of-the-art solid state battery (SSB) processing technique based on tape-casting and co-firing techniques limits the further improvement of energy density and power density because the single cells need thick component layers to provide mechanical strength. Furthermore, each component layer's different heat processing conditions make it impossible to manufacture the high-density high-compact multilayer (HCML) SSB using the rapid additive manufacturing (RAM) technique. Therefore, the project is to develop a new processing method for fabricating SSB electrolyte thin films with well-controlled composition, crystal structure, microstructure, and thickness to achieve high-performance battery electrolytes to enable the RAM of HCML-SSBs. The project's overarching goal is to improve the battery's essential properties of energy density, power, packaging design, safety, and scalability to help NASA's all-electric vertical take-off and landing vehicles (eVTOL) technology. The project is to serve as a bridge to establish a partnership between NASA LaRC and Clemson University based on the research area of Appendix G: NASA ARMD Electric Aircraft Batteries & Crash Safety Research-Materials and Processes for All-Solid-State Batteries for Electric Aircraft. The project technical objective is to develop a rapid laser reactive sintering method for fabricating fully dense SSB electrolyte (e.g., doped Li7La3Zr2O12) thin films with well-controlled thickness, composition, crystal structure, and microstructure to achieve high-performance SSB electrolytes, providing a prerequisite knowledge for rapid additive manufacturing of practical HCML-SSBs. By leveraging our RLRS method for the controllable-processing of protonic ceramics, we designed the RLRS experiment for processing doped LLZO thin films with the desired properties. The RLRS method consists of three steps: 1) preparation of paste/slurry, 2) 3D printing of thin green films, and 3) CO2 laser scanning to achieve final films. The printable pastes or slurries of doped LLZO precursors can come from the cost-effective raw materials of oxides and carbonates through conventional ball-milling and vacuum-mixing. The 3D printing techniques based on microextrusion (ME) and ultrasonic spray coating (USC) can deposit doped LLZO green films with designed thickness. The CO2 laser scanning on the top of the electrolyte precursor green films can achieve the final electrolyte thin films on the pre-selected substrates. The optimization of organic additives and sintering aid to electrolyte precursor mixture and the optimization of laser sintering parameters allow us to achieve electrolyte thin films with the desired thickness, crystal structure, microstructure, and complete density. The additional thermodynamic driving force of the chemical reaction and the liquid sintering due to proper sintering aids are the two factors that ensure crack-free electrolytes and complete dense film with the desired microstructure. The proposed technology has several advantages. 1) To start from raw materials of oxides and carbonates decreases the materials cost and simplifies the processing. 2) The ME and USC-based 3D printing can manufacture thin green layers with the desired thickness, and geometry complexity can directly contribute to the RAM of SSBs. 3) The rapid and facile laser scanning combines phase formation, chemical reaction, densification, microstructure control, and geometry adjustment in one facile laser scan step. 4) The selective laser sintering processes green films with precise in-plane (X-Y) and out-of-plane (Z) position to achieve well-distributed structures. 5) The rapid in-situ consolidation of green ceramic layers makes it possible for rapid additive manufacturing of SSBs. 6) The large adjustment window of material additives and laser processing parameters allows the control of the ceramic oxide relative density and morphology, extending the application to the porous electrode for SSB manufacturing.

This is a mature technology (TRL 7+) — the realistic path in is usually NASA's Technology Transfer Program: licensing an existing NASA patent, or a Space Act Agreement to use NASA facilities/expertise directly. NASA also runs a startup licensing program with no upfront fee for companies formed to commercialize a specific NASA technology.

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