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

作者：Yu, Chuang; Ganapathy, Swapna; Van Eck, Ernst R. H.; Wang, Heng; Basak, Shibabrata; Li, Zhaolong; Wagemaker, Marnix^*

来源：Nature Communications, 2017, 8(1): 1086.

DOI：10.1038/s41467-017-01187-y

• ELECTROCHEMICAL PERFORMANCE
• ARGYRODITE LI6PS5CL
• SECONDARY BATTERIES
• RECENT PROGRESS
• CONDUCTORS
• STABILITY
• DIFFUSION
• TIO2
• NANOARCHITECTONICS
• LIMN2O4

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.

• 出版日期2017-10-20