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A three-dimensional vertical-aligned graphene-polydopamine electrode (PDA@3DVAG) composite with vertical channels and conductive network is prepared by a method of unidirectional freezing and subsequent self-polymerization. When the prepared PDA@3DVAG is constructed as the positive electrode of zinc-ion hybrid supercapacitors (ZHSCs), excellent electrochemical performances are obtained. Compared with the conventional electrolyte, PDA@3DVAG composite electrode in highly concentrated salt electrolyte exhibits better multiplicity performance (48.92% at a current density of 3 A g−1), wider voltage window (−0.8~0.8 V), better cycle performance with specific capacitance from 96.7 to 59.8 F g−1, and higher energy density (46.14 Wh kg−1).

Aqueous Organic Zinc-Ion Hybrid Supercapacitors Prepared by 3D Vertically Aligned Graphene-Polydopamine Composite Electrode