TY - JOUR
T1 - Accessing the bottleneck in all-solid state batteries, lithium-ion transport over the solid-electrolyte-electrode interface
AU - Yu, Chuang
AU - Ganapathy, Swapna
AU - van Eck, Ernst R H
AU - Wang, Heng
AU - Basak, Shibabrata
AU - Li, Zhaolong
AU - Wagemaker, Marnix
PY - 2017/12/1
Y1 - 2017/12/1
N2 - 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.
AB - 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.
KW - batteries
KW - Solid-state NMR
UR - http://resolver.tudelft.nl/uuid:573f2a72-1ef1-4831-a3b5-979d71e55abe
UR - http://www.scopus.com/inward/record.url?scp=85032207301&partnerID=8YFLogxK
U2 - 10.1038/s41467-017-01187-y
DO - 10.1038/s41467-017-01187-y
M3 - Article
AN - SCOPUS:85032207301
SN - 2041-1723
VL - 8
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 1086
ER -