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HighlightsA surface engineering strategy was proposed to design hierarchically porous structure on fibrous carbon cathodes with O/N heteroatom functional groups.    High-energy and anti-self-discharge Zn-ion hybrid supercapacitors (ZHSs) were realized.    ZHS electrochemistry was investigated and new insights were provided.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-021-00625-3.

Towards High-Energy and Anti-Self-Discharge Zn-Ion Hybrid Supercapacitors with New Understanding of the Electrochemistry