Imaging the charge and discharge of solid-state batteries

Significance 

The lithium-ion batteries now in widespread use for everything from mobile electronics to electric vehicles rely on a liquid electrolyte to carry ions back and forth between electrodes within the battery during charge and discharge cycles. The liquid uniformly coats the electrodes, allowing free movement of the ions. Rapidly-evolving solid state battery technology instead uses a solid electrolyte, which should help boost energy density and improve the safety of future batteries. But removal of lithium from electrodes can create voids at interfaces that cause reliability issues that limit how long the batteries can operate. To counter this, creating structured interfaces through different deposition processes will be required to try to maintain contact through the cycling process. Precise control and engineering of these interface structures will be very important for future solid-state battery development and  design interfaces.

The Georgia Tech research team led by Matthew McDowell, an assistant professor in the George W. Woodruff School of Mechanical Engineering and the School of Materials Science and Engineering built special test cells about two millimeters wide which were designed to be studied at the Advanced Photon Source, a synchrotron facility at Argonne National Laboratory, a U.S. Department of Energy Office of Science facility located near Chicago. The authors studied the changes in battery structure during a five-day period of intensive experiments. The instrument takes images from different directions, and you reconstruct them using computer algorithms to provide 3-D images of the batteries over time.

Using X-ray tomography, a research team has observed the internal evolution of the materials inside solid-state lithium batteries as they were charged and discharged. Detailed three-dimensional information from the research could help improve the reliability and performance of the batteries, which use solid materials to replace the flammable liquid electrolytes in existing lithium-ion batteries.

The operando synchrotron X-ray computed microtomography imaging revealed how the dynamic changes of electrode materials at lithium/solid-electrolyte interfaces determine the behavior of solid-state batteries. The researchers found that battery operation caused voids to form at the interface, which created a loss of contact that was the primary cause of failure in the cells. The findings provides fundamental understanding of what is happening inside the battery, and that information should be important for guiding engineering efforts that will push these batteries closer to commercial reality in the next several years. The research work is now published in journal Nature Materials.

Because of limitations in the testing, the researchers were only able to observe the structure of the batteries through a single cycle. In future work, the research team would like to see what happens over additional cycles, and whether the structure somehow adapts to the creation and filling of voids. They believe the results would likely apply to other electrolyte formulations, and that the characterization technique could be used to obtain information about other battery processes. Battery packs for electric vehicles must withstand at least a thousand cycles during a projected 150,000-mile lifetime. While solid-state batteries with lithium metal electrodes can offer more energy for a given size battery, that advantage won’t overcome existing technology unless they can provide comparable lifetimes. The study should help advance this technology toward broader commercial applications

Imaging the charge and discharge of solid-state batteries - Advances in Engineering
Solid-state batteries are charged and discharged in custom-made hardware designed at Georgia Tech. A smaller, modified version of the cell shown here was used to image these materials during cycling. Credit: Matthew McDowell, Georgia Tech.
Imaging the charge and discharge of solid-state batteries - Advances in Engineering
A three-dimensional view of the lithium/solid-electrolyte interface within the battery reconstructed with X-ray tomography. Credit: Matthew McDowell, Georgia Tech

About the author

Matthew McDowell
Assistant Professor

Dr. Matthew McDowell joined Georgia Tech in the fall of 2015 as an assistant professor with a joint appointment in the George W. Woodruff School of Mechanical Engineering and the School of Materials Science and Engineering. Prior to this appointment, he was a postdoctoral scholar in the Division of Chemistry and Chemical Engineering at the California Institute of Technology. Dr. McDowell received his Ph.D. in 2013 from the Department of Materials Science and Engineering at Stanford University.

Dr. McDowell’s research group focuses on understanding how materials for energy and electronic devices change and transform during operation, and how these transformations impact properties. The group uses in situ experimental techniques to probe materials transformations under realistic conditions. The fundamental scientific advances made by the group guide the engineering of materials for breakthrough new devices.

Current projects in the group are focused on i) electrode materials for alkali ion batteries, ii) materials for solid-state batteries, iii) interfaces in chalcogenide materials for electronics and catalysis, and iv) new methods for creating nanostructured metals.

Reference

John A. Lewis, Francisco Javier Quintero Cortes, Yuhgene Liu, John C. Miers, Ankit Verma, Bairav S. Vishnugopi, Jared Tippens, Dhruv Prakash, Thomas S. Marchese, Sang Yun Han, Chanhee Lee, Pralav P. Shetty, Hyun-Wook Lee, Pavel Shevchenko, Francesco De Carlo, Christopher Saldana, Partha P. Mukherjee & Matthew T. McDowell. Linking void and interphase evolution to electrochemistry in solid-state batteries using operando X-ray tomography. Nature Materials (2021)

Go To Nature Materials

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