Accessing the bottleneck in all-solid state batteries, lithium-ion transport over the solid-electrolyte-electrode interface

Chuang Yu, Swapna Ganapathy, Ernst R. H. van Eck, Heng Wang, Shibabrata Basak, Zhaolong Li and Marnix Wagemaker ()
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Chuang Yu: Delft University of Technology
Swapna Ganapathy: Delft University of Technology
Ernst R. H. van Eck: Radboud University
Heng Wang: Delft University of Technology
Shibabrata Basak: Delft University of Technology
Zhaolong Li: Delft University of Technology
Marnix Wagemaker: Delft University of Technology

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: Abstract Solid-state batteries potentially offer increased lithium-ion battery energy density and safety as required for large-scale production of electrical vehicles. One of the key challenges toward high-performance solid-state batteries is the large impedance posed by the electrode–electrolyte interface. However, direct assessment of the lithium-ion transport across realistic electrode–electrolyte interfaces is tedious. Here we report two-dimensional lithium-ion exchange NMR accessing the spontaneous lithium-ion transport, providing insight on the influence of electrode preparation and battery cycling on the lithium-ion transport over the interface between an argyrodite solid-electrolyte and a sulfide electrode. Interfacial conductivity is shown to depend strongly on the preparation method and demonstrated to drop dramatically after a few electrochemical (dis)charge cycles due to both losses in interfacial contact and increased diffusional barriers. The reported exchange NMR facilitates non-invasive and selective measurement of lithium-ion interfacial transport, providing insight that can guide the electrolyte–electrode interface design for future all-solid-state batteries.

Date: 2017
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DOI: 10.1038/s41467-017-01187-y

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