Abstract
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A novel flexible three-dimensional (3D)
architecture of nitrogen and sulfur codoped graphene has
been successfully synthesized via thermal treatment of a liquid
crystalline graphene oxide−doping agent composition, followed
by a soft self-assembly approach. The high temperature
process turns the layer-by-layer assembly into a high surface
area macro- and nanoporous free-standing material with
different atomic configurations of graphene. The interconnected
3D network exhibits excellent charge capacitive performance of 305 F g−1 (at 100 mV s−1), an unprecedented volumetric
capacitance of 188 F cm−3 (at 1 A g−1), and outstanding energy density of 28.44 Wh kg−1 as well as cycle life of 10 000 cycles as a
free-standing electrode for an aqueous electrolyte, symmetric supercapacitor device. Moreover, the resulting nitrogen/sulfur
doped graphene architecture shows good electrocatalytic performance, long durability, and high selectivity when they are used as
metal-free catalyst for the oxygen reduction reaction. This study demonstrates an efficient approach for the development of
multifunctional as well as flexible 3D architectures for a series of heteroatom-doped graphene frameworks for modern energy
storage as well as energy source applications.