Scalable 2D Hierarchical Porous Carbon Nanosheets for Flexible Supercapacitors with Ultrahigh Energy Density

Abstract

2D carbon nanomaterials such as graphene and its derivatives, have gained tremendous research interests in energy storage because of their high capacitance and chemical stability. However, scalable synthesis of ultrathin carbon nanosheets with well-defined pore architectures remains a great challenge. Herein, the first synthesis of 2D hierarchical porous carbon nanosheets (2D-HPCs) with rich nitrogen dopants is reported, which is prepared with high scalability through a rapid polymerization of a nitrogen-containing thermoset and a subsequent one-step pyrolysis and activation into 2D porous nanosheets. 2D-HPCs, which are typically 1.5 nm thick and 1–3 µm wide, show a high surface area (2406 m² g⁻¹) and with hierarchical micro-, meso-, and macropores. This 2D and hierarchical porous structure leads to robust flexibility and good energy-storage capability, being 139 Wh kg⁻¹ for a symmetric supercapacitor. Flexible supercapacitor devices fabricated by these 2D-HPCs also present an ultrahigh volumetric energy density of 8.4 mWh cm⁻³ at a power density of 24.9 mW cm⁻³, which is retained at 80% even when the power density is increased by 20-fold. The devices show very high electrochemical life (96% retention after 10000 charge/discharge cycles) and excellent mechanical flexibility.

2D hierarchical porous carbon nanosheets (2D-HPCs) are prepared by a one-step carbonization and activation of a p-phenylenediamine-acetaldehyde resin which is synthesized via a one-pot scalable polymerization. 2D-HPCs, which are of 1.5 nm thickness, 1–3 µm wide, ultrarich porosity with hierarchical pore distribution, are used to fabricate flexible supercapacitors with high gravimetric and volumetric energy densities, as well as excellent mechanical flexibility.

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