Overcoming volumetric capacitance-rate performance tradeoff with 0D/2D conductive carbon nitride/phosphorene heterostructure for flexible supercapacitor

Few-layer black phosphorus (FL-BP) is considered a rising star 2D material for flexible supercapacitors (FSCs) due to its exceptional properties, including mechanical flexibility and high active surface area. However, the disordered deposition of FL-BP nanoflakes often leads to face-to-face restacking, which diminishes the effective active area and ion transport channels. This poses a huge challenge in simultaneously achieving high volumetric capacitance and rate capability. To address this, a 3D porous 0D/2D FL-BP/conductive carbon nitride (FL-BP/cCN) film has been developed. The introduction of 0D c-CN nanoparticles effectively prevents the restacking of FLBP nanoflakes and expands the nanofluidic channels, thus facilitating charge transport and ions diffusion. Additionally, the highly conductive c-CN nanoparticles embedded into the FL-BP layers significantly improve overall conductivity. As a result, the FL-BP/c-CN film-based FSC demonstrates a remarkable rate performance, retaining 70% capacitance as the scan rate increases from 10 to 100 mV/s. Moreover, the incorporation of 0D cCN nanoparticles increases the available space for charge accumulation, yielding a volumetric capacitance of 28.5 F/cm3 at a scan rate of 10 mV/s, which is three times higher than that of a pure FL-BP film electrode (9.2 F/ cm3). This work presents an innovative approach for developing high-performance FL-BP-based FSCs.