TY  - JOUR
PY  - 2023//
TI  - Mechanical regulation of lithium intrusion probability in garnet solid electrolytes
JO  - Nature energy
A1  - Xu, Xin
A1  - McConohy, Geoff
A1  - Cui, Teng
A1  - Barks, Edward
A1  - Wang, Sunny
A1  - Kaeli, Emma
A1  - Melamed, Celeste
A1  - Gu, X. Wendy
A1  - Chueh, William C.
SP  - ePub
EP  - ePub
VL  - ePub
IS  - ePub
N2  - Solid electrolytes in rechargeable lithium-metal batteries are susceptible to lithium-metal short circuiting during plating, and the root cause is under debate. In this work, we investigated statistically the effect of locally and globally applied stress on lithium penetration initiation in Li6.6La3Ta0.4Zr1.6O12 (LLZO) via operando microprobe scanning electron microscopy. Statistical analysis revealed that the cumulative probability of intrusion as a function of lithium-metal diameter follows a Weibull distribution. Upon increasing the microprobe-LLZO contact force, the characteristic failure diameter of lithium metal decreases significantly. In addition, we control the direction of intrusion propagation by applying a 0.070% compressive strain via operando cantilever beam-bending experiments. Overall, we find that the root cause of lithium intrusion into the electrolyte is a combination of current focusing and the presence of nanoscale cracks, rather than electronic leakage or electrochemical reduction. These insights highlight the mechanical tunability of electrochemical plating reactions in brittle solid electrolytes.<p />  <p>Language: en</p>
LA  - en
SN  - 2058-7546
UR  - http://dx.doi.org/10.1038/s41560-022-01186-4
ID  - ref1
ER  -