Abstract

Safety and lifespan problems caused by the zinc dendrite formation continue to impede the application of zinc-based batteries. To address this severe issue, it is crucial to fully understand the nanoscale nucleation and early-stage dendrite growth process. However, the key dynamic process can hardly be resolved at the nanoscopic level under ambient working conditions with the current in situ / operando methods. Here, we develop a highly sensitive, super-resolution operando imaging approach for directly investigating the initial electroplating process in the zinc-air battery system. With this approach, millisecond/nanometer-resolution observation is achieved, providing nucleation rate, growth heterogeneity, and direction information at the single zinc nuclei level, and revealing nanoscopic details of early-stage dendrite growth. The spatiotemporally super-resolved observation elucidates that dynamic change in the local electrochemical environment is the key factor for the formation of the zinc dendrites. This novel straightforward approach can enable a deep understanding of the electrochemical interfacial issues and facilitate problem solving in diverse battery systems. Super-resolution operando imaging of zinc initial electroplating process Millisecond/nanometer resolution observation of single zinc nuclei formation Zinc nucleation rate, growth heterogeneity, and direction obtained Super-resolved early-stage dendrites formation and role of zinc depletion In-depth understanding of initial electroplating dynamics is crucial for designing/developing safer batteries. Here, Ye et al. develop a super-resolution microscopy with nanoscale and millisecond resolution, that enables the direct imaging and analysis of highly dynamic zinc nucleation and early-stage dendrite growth under ambient conditions. This new approach can be used for probing key interfacial electrochemical issues in diverse battery systems.

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