Curved Fragmented Graphenic Hierarchical Architectures for Extraordinary Charging Capacities

An approach to assemble hierarchically ordered 3D arrangements of curved graphenic nanofragments for energy storage devices is described. Assembling them into well‐defined interconnected macroporous networks, followed by removal of the template, results in spherical macroporous, mesoporous, and microporous carbon microball (3MCM) architectures with controllable features spanning nanometer to micrometer length scales. These structures are ideal porous electrodes and can serve as lithium‐ion battery (LIB) anodes as well as capacitive deionization (CDI) devices. The LIBs exhibit high reversible capacity (up to 1335 mAh g−1), with great rate capability (248 mAh g−1 at 20 C) and a long cycle life (60 cycles). For CDI, the curved graphenic networks have superior electrosorption capacity (i.e., 5.17 mg g−1 in 0.5 × 10−3m NaCl) over conventional carbon materials. The performance of these materials is attributed to the hierarchical structure of the graphenic electrode, which enables faster ion diffusion and low transport resistance. Unambiguous formation of a graphene nanofragment with the advantage of curved architecture with high‐surface area 3D mesostructure offers low‐tortuosity electrode architectures containing fast ion diffusion pathways and low transport resistance. A rare macroporous curved graphene framework formed via evaporation‐induced self‐assembly is an illusion that demonstrates extraordinary charging capacity as 3MCM–assembled anode for lithium‐ion batteries (LIBs) and capacitive deionization (CDI).