Analytical Observation of Cathodic Zinc Deposition in High-Capacity Zinc Oxide Electrodes for Rechargeable Zinc-based Batteries: Influence of the Current Rate in the First Charging

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The effects of the current rate used during the first charging (pre-charging: so-called “formation”) on the cathodic deposition of metallic zinc (Zn) were analyzed for the high capacity (thick) zinc oxide (ZnO) electrode in rechargeable Zn-based batteries. Pre-charging at a lower current rate (1.875 mA cm⁻²) enabled greater electrode performances for the subsequent charge-discharge cycles. The Zn deposition profiles were investigated by conventional postmortem X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopy using a scanning electron microscope, as well as in situ synchrotron XRD and ex situ synchrotron X-ray computed tomography. The results revealed significant differences in the deposition profiles of the metallic Zn depending on the current rates used during pre-charging. The higher rate (18.75 mA cm⁻²) resulted in an inhomogeneous deposition of Zn, whereas the lower rate yielded finer Zn particles dispersed homogeneously throughout the thick ZnO electrode. These morphological and spatial variations in the Zn deposition during pre-charging affected the subsequent cycling behavior of the thick ZnO electrode.