Accessing the bottleneck in all-solid state batteries, lithium-ion transport over the solid-electrolyte-electrode interface
Chuang Yu (TU Delft - RST/Fundamental Aspects of Materials and Energy)
Swapna Ganapathy (TU Delft - RST/Fundamental Aspects of Materials and Energy)
Ernst R H van Eck (Radboud Universiteit Nijmegen)
Heng Wang (TU Delft - RST/Fundamental Aspects of Materials and Energy)
Shibabrata Basak (TU Delft - QN/Zandbergen Lab, Kavli institute of nanoscience Delft)
Zhaolong Li (TU Delft - RST/Fundamental Aspects of Materials and Energy)
Marnix Wagemaker (TU Delft - RST/Fundamental Aspects of Materials and Energy)
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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.