Linking the Defects to the Formation and Growth of Li Dendrite in All-Solid-State Batteries

The nucleation and growth of Li metal during deposition and the associated dendrite penetration are the critical and fundamental issues influencing the safety and power density of solid-state lithium metal batteries (SSLBs). However, investigations on Li metal deposition/dissolution especially the formation and growth of Li dendrites and their determining factors in the all-solid-state electrochemical systems are still lacking. In this work, in situ observations of the Li metal growth process, and defects induced heterogeneous deposition under cathodic load, are reported. By exploiting in situ scanning electron microscopy, along with electrochemical analytical approaches, the spatial distribution and morphological evolution of the deposited Li at the electrode|solid electrolyte interface are obtained and discussed. This investigation reveals that the formation of lithium whiskers is decided by the local Li ion flux and the deposition active sites, which are closely dependent on the content and types of defects in the polycrystalline electrolyte. Moreover, the defect regions exhibit faster Li deposition kinetics and higher nucleation tendency. These results can advance the fundamental understanding of the Li penetration mechanism in SSLBs.

Automated summary

This study reveals the issues of heterogeneous deposition of defects during the growth process of lithium metal through in situ observation and electrochemical analytical methods, demonstrating the relationship between the formation of lithium whiskers and the local lithium ion flux and active sites, as well as the association of these active sites with defects in polycrystalline electrolyte.