Publication date: 10th April 2024
Lithium metal solid state batteries (SSB) have the potential to increase energy density while substantially improving safety of operation for lithium-ion-transport battery technology. However these improvements remain largely theoretical due to two dominant failure pathways: interfacial voiding between the Li anode and the ceramic electrolyte during stripping, and the penetration of Li metal dendrites through the ceramic during plating. To mitigate these issues a Critical Current Density (CCD) has been identified, below which the battery can be safely cycled, to the detriment of overall battery performance. It is thought that void formation during anode stripping promotes subsequent dendrite formation during plating, making the voiding problem a primary obstacle to increased SSB performance. Previous theoretical work [1] has identified deficiencies in prevailing theories for the driving forces behind interfacial voiding, inhibiting fundamental understanding for the problem and consequently the identification of solutions. Until now all experimental evidence for interfacial voiding has been post-mortem and observed destructively, so that these theories could not yet be validated. To do so, we have performed in-situ void closure experiments with intentional cylindrical voids placed at the interface of a Li-LLZO (Li6.6Ta0.4La3Zr1.6O12)-Li cell. With our approach, in-situ observation of discrete and intentional interfacial voids has allowed for confirmation of rapid and predictable void collapse under three distinct environments: 1) purely mechanical compressive loading, 2) purely electro-chemical stripping current, and 3) both stripping current and applied stack pressure. Void shrinkage and closure, dictated by power-law creep governing the Li anode and Butler-Volmer kinetics governing the Li ion transport physics, suggests that the issue of interfacial voiding leading to eventual contact loss of the anode during battery operation is governed by phenomena that may be wholly distinct from these fundamental theories. Conventional thinking on void formation therefore cannot justify the contact loss phenomenon plaguing SSB performance.
This work was supported by the Faraday Institution [FutureCat grant number FIRG017 and Degredation years 4-5 grant number FIRG024].
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