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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.
Highlights
Solid-state batteries potentially offer increased lithium-ion battery energy density and safety as required for large-scale production of electrical vehicles
The argyrodite Li6PS5Br solid electrolyte material was prepared by ball milling at 600 rpm for different milling times followed by annealing at 300 °C for 5 h
Nuclear magnetic resonance (NMR), which probes the lithium-ion hopping through the bulk lattice, resulted in a conductivity of 0.013(1) S cm−1 at 78 °C with an activation energy of 0.10(5) eV, indicating mobility comparable with recently reported NMR results[51], and a larger bulk conductivity than that resulting from impedance spectroscopy
Summary
Solid-state batteries potentially offer increased lithium-ion battery energy density and safety as required for large-scale production of electrical vehicles. Perhaps one of the biggest challenges is the mechanical stability, where the volume changes of electrode materials during (dis)charge may cause loss of contact between the electrode and the electrolyte particles, blocking lithium-ion transport across the interface These challenges indicate that whether or not solid-state batteries will be able to deliver the performance necessary for EVs will depend on the development of stable interfaces that allow facile ionic charge transfer. An additional opportunity provided by solid-state NMR in multi-phase battery materials, either consisting of multiple electrode phases or a mixture of electrode and electrolyte phases, is the possibility to measure the spontaneous lithium-ion exchange between different lithium-containing phases This provides unique selectivity for charge transfer over phase boundaries[24, 47, 49], as recently shown to be feasible for the Li6PS5Cl–Li2S solid electrolyte–electrode combination[24]
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