Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries

Cheng, Zhu; Liu, M.; Ganapathy, S.; Li, Z.; Zhang, Xiaoyu; He, Ping; Zhou, Haoshen; Wagemaker, M.; Li, Chau

doi:10.1016/j.joule.2020.04.002

Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries

Title

Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries

Author

Cheng, Zhu (Nanjing University)
Liu, M. (TU Delft RST/Storage of Electrochemical Energy)
Ganapathy, S. (TU Delft RID/TS/Instrumenten groep)
Li, Z. (TU Delft RST/Storage of Electrochemical Energy)
Zhang, Xiaoyu (Nanjing University)
He, Ping (Nanjing University)
Zhou, Haoshen (Nanjing University; National Institute of Advanced Industrial Science and Technology (AIST))
Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy)
Li, Chau (Nanjing University)

Date

2020

Abstract

The influence of space-charge layers on the ionic charge transport over cathode-solid electrolyte interfaces in all-solid-state batteries remains unclear because of the difficulty to unravel it from other contributions to the ion transport over the interfaces. Here, we reveal the effect of the space-charge layers by systematically tuning the space-charge layer on and off between Li _xV ₂O ₅ and Li _1.5Al _0.5Ge _1.5(PO ₃) ₄ (LAGP), by changing the Li _xV ₂O ₅ potential and selectively measuring the ion transport over the interface by two-dimensional (2D) NMR exchange. The activation energy is demonstrated to be 0.315 eV for lithium-ion exchange over the space-charge-free interface, which increases dramatically to 0.515 eV for the interface with a space-charge layer. Comparison with a space-charge model indicates that the charge distribution due to the space-charge layer is responsible for the increased interface resistance. Thereby, the present work provides selective and quantitative insight into the effect of space-charge layers over electrode-electrolyte interfaces on ionic transport.