3D-PRintable glass-based Electrolytes for all-Solid-State lithium batteries

Project Information

3D-PRESS

Grant agreement ID: 841937

DOI

10.3030/841937

Project closed

EC signature date 30 April 2019

Start date 2 March 2020

End date 31 May 2022

Funded under

• EXCELLENT SCIENCE - Marie Skłodowska-Curie Actions

Total cost

€ 160 932,48

EU contribution

€ 160 932,48

Coordinated by

FUNDACIO INSTITUT DE RECERCA EN ENERGIA DE CATALUNYA
Spain

Periodic Reporting for period 1 - 3D-PRESS (3D-PRintable glass-based Electrolytes for all-Solid-State lithium batteries)

Reporting period: 2020-03-02 to 2022-03-01

Summary of the context and overall objectives of the project

The main goal of the 3D-PRESS project was to advance on the 3D printing concepts for safer, cheaper and customizable all-solid state Li batteries (ASSLB). More specifically, the project focused on the design, production, characterization and testing of 3D printed NASICON-type glass-based electrolytes for 3D printed batteries.

3D-PRESS represents a cutting edge multidisciplinary approach for the development of reliable and customizable all-solid state 3D ASSLB, especially interesting for micro-power applications such as for the Internet of Things (IoT). The project provided a new family of printable materials increasing the short list of available compositions, especially solid electrolytes, opening the door to the development of a new generation of fully printable all-solid state 3D batteries with complex architectures.

In 3D-PRESS we were able to print Li1.5Al0.5Ge1.5(PO4)3 (LAGP) with two different techniques: robocasting and stereolitography. The complex geometries obtained allowed an increase in the effective area of the electrolyte directly related to a decrease in the area specific resistance of the component. This will allow the production of the next generation of ASSLB with improved energy density. A peer-reviewed paper reporting the main outcomes of the project has been submitted and will soon be available.

The project was carried out by Gianfranco Sabato, who worked in the Nanoionics and Fuel Cells group at IREC since March 2020 until May 2022, thanks to an IF-MSCA-H2020 fellowship.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

As first task in 3D-PRESS commercial amorphous LAGP was characterized in order to optimize a sinter-crystallization thermal treatment, with the main objective to achieve high degree of densification avoiding detrimental reaction or degradation of the material.
As following step, two different 3D printing techniques were considered: Robocasting and Stereolitography. The formulation of ceramic containing pastes were optimized for the two processes, as well as the printing parameters. With both the techniques it was possible to achieve complex LAGP structures with increased interfacial area with the electrodes. Finally the 3D-printed electrolytes were electrochemically characterized by means of electrochemical impedance spectroscopy and chronopotentiometry (in symmetrical cells Li/LAGP/Li).

The use of 3D printing techniques allowed the fabrication of simple as well as complex architectures, with enhanced contact area with the electrodes. The inks and the printing processes were both optimized in order to reach an accuracy up to ≈100 µm. The printed structures demonstrated an excellent densification after the firing/sintering treatment, as a result of the optimization of the inks formulation, printing process and sintering conditions. Furthermore, ionic conductivity of 3D-printed LAGP electrolyte resulted to be 1.8 10-4 S cm-1 at room temperature, in accordance with the values measured on the same material processed with conventional methods. No detrimental reaction products or degradation phenomena were detected by chemical analyses after the sintering.

A peer-reviewed paper reporting the main outcomes of the project has been submitted and will soon be available. In addition, the collected results were presented in top international conferences on materials science and technology: such as EMRS spring meeting and ICACC22.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

3D-PRESS represented a completely new approach in comparison with the state of the art manufacturing of ceramic electrolytes for Lithium batteries. For the first time the direct 3D-printing of full-ceramic Nasicon-type electrolyte was reported. In addition, the production of complex shaped geometries demonstrated as proof of concept the possibility to decrease the area specific resistance of the electrolytes thanks to new design feasible via additive manufacturing.
The results obtained in 3D-PRESS open the door to a complete new approach for the next generation full ceramic Lithium batteries. Allowing to overcome the limits and drawback related to the use of liquid electrolytes.

3D printed interdigitated LAGP solid electrolytes