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

Zhu Cheng, Ming Liu, Swapna Ganapathy, Zhaolong Li, Xiaoyu Zhang, Ping He*, Haoshen Zhou, Marnix Wagemaker, Chau Li

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

32 Citations (Scopus)
15 Downloads (Pure)

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.

Original languageEnglish
Pages (from-to)1311-1323
Number of pages13
JournalJoule
Volume4
Issue number6
DOIs
Publication statusPublished - 2020

Keywords

  • 2D exchange NMR
  • interfaces
  • LAGP
  • Li-ion diffusion
  • LiVO
  • solid-state batteries
  • space-charge layers

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