A key to improve the electrochemical performance of energy storage systems (e.g., lithium ion batteries and supercapacitors) is to develop advanced electrode materials. In the last few years, although originating from the unique structure and property of graphene, interest has expanded beyond the originally literally defined graphene into versatile integration of numerous intermediate structures lying between graphene and organic polymer, particularly for the development of new electrode materials for energy storage devices. Notably, diverse designations have shaded common characteristics of the molecular configurations of these newly-emerging materials, severely impeding the design, synthesis, tailoring, functionalization, and control of functional electrode materials in a rational and systematical manner. This concept paper highlights all these intermediate materials, specifically comprising graphene subunits intrinsically interconnected by organic linkers or fractions, following a general concept of graphenal polymers. Combined with recent advances made by our group and others, two representative synthesis approaches (bottom-up and top-down) for graphenal polymers are outlined, as well as the structure-property relationships of these graphenal polymers as energy storage electrode materials are discussed.
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