▎ 摘　　要

We proved that ice crystallized from water molecules within as-synthesized graphene oxide (GO) can be used as a spacer among individual GO sheets to form an expanded GO aerogel with a three-dimensional porous network structure. This designed specific structure can be retained during further processes to form graphene paper. Due to the fact that the as-fabricated graphene paper contains carbon defects and space in its infrastructure, this creates more electroactive surfaces and interfaces to significantly increase the Faradaic reaction efficiency. With the introduction of redox-electrolyte K3Fe(CN)(6) into a KOH electrolyte, we can obtain a 95-fold increase in the specific capacitance compared with the value obtained in the traditional KOH electrolyte. The ice-crystallization formed graphene paper electrode showed high electro-activity because the specific porous structure can favor the fast transfer of electrolyte ions, such as Fe(CN)(6)(3-) ions. The presented results prove that ice-crystallization formed GO can serve as a chemically tunable platform for electrochemical energy storage applications.