Progressive and instantaneous nature of lithium nucleation discovered by dynamic and operando imaging

The understanding of lithium (Li) nucleation and growth is important to design better electrodes for high-performance batteries. However, the study of Li nucleation process is still limited because of the lack of imaging tools that can provide information of the entire dynamic process. We developed and used an operando reflection interference microscope (RIM) that enables real-time imaging and tracking the Li nucleation dynamics at a single nanoparticle level. This dynamic and operando imaging platform provides us with critical capabilities to continuously monitor and study the Li nucleation process. We find that the formation of initial Li nuclei is not at the exact same time point, and Li nucleation process shows the properties of both progressive and instantaneous nucleation. In addition, the RIM allows us to track the individual Li nucleus's growth and extract spatially resolved overpotential map. The nonuniform overpotential map indicates that the localized electrochemical environments substantially influence the Li nucleation.

Automated summary

Understanding the nucleation and growth of lithium (Li) is crucial for designing high-performance battery electrodes. However, limited research has been done on the Li nucleation process due to a lack of imaging tools that can provide information on the entire dynamic process. We developed and utilized an operando reflection interference microscope (RIM) to achieve real-time imaging and tracking of Li nucleation dynamics at the individual nanoparticle level. This dynamic and operando imaging platform gives us the essential capabilities to continuously monitor and study the Li nucleation process. Our findings reveal that the formation of initial Li nuclei does not occur at the exact same time, and the Li nucleation process exhibits properties of both progressive and instantaneous nucleation. Furthermore, the RIM allows us to track the growth of individual Li nuclei and extract spatially resolved overpotential maps, which indicate that localized electrochemical environments significantly influence Li nucleation.