Through the calculation of the Gibbs free energy of the hydrogen evolution reaction (HER) process, the association of cathode by-products with voltage windows was described and confirmed for the first time: whether the by-product layer on the surface of the cathode material is broken or not can be considered a criterion for selecting the voltage window. Herein, the protective effect of by-products deposited on the surface structure of the cathode material was studied based on the differences in the cycling stability of ultrathin carbon materials (UTCs) at different voltage windows. However, the selection of the voltage window to achieve the balance between energy density and cycling stability is still difficult. Aqueous zinc-ion hybrid supercapacitors (ZHSs) are promising energy storage devices owing to their high energy and power density.
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