Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries
Zhu Cheng (Nanjing University)
Ming Liu (TU Delft - RST/Storage of Electrochemical Energy)
Swapna Ganapathy (TU Delft - RID/TS/Instrumenten groep)
Zhaolong Li (TU Delft - RST/Storage of Electrochemical Energy)
Xiaoyu Zhang (Nanjing University)
Ping He (Nanjing University)
Haoshen Zhou (Nanjing University, National Institute of Advanced Industrial Science and Technology (AIST))
Marnix Wagemaker (TU Delft - RST/Storage of Electrochemical Energy)
Chau Li (Nanjing University)
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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.
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