Nitrogen-doped graphene forests as electrodes for high-performance wearable supercapacitors

Highlights: •N-doped graphene forest (GF) is successfully synthesized by in-situ PECVD process. •Morphology of N-doped GF electrode realizes a better in-plane electron transfer. •Areal and volumetric capacitances increase 26% and 89% by the N-doping of GF. •Energy and power densities increase 87% and 50% by the N-doping of GF. •The N-doped GF-based EDLC shows excellent bendability and reliable durability. -- Abstract: Recently, a graphene forest (GF) is synthesized by a plasma enhanced chemical vapor deposition (PECVD) process, which subverts the stereotyped morphology of vertical graphene. The GF is demonstrated to possess excellent performance in flexible and bendable electrical double-layer capacitors (EDLCs). In this work, synthesis process of the GF has been optimized and N-doped GF is successfully achieved by introducing NH₃ as the nitrogen precursor during the PECVD process. The N-doping obviously affects the morphology of the GF and the in-plane conductivity of GF is desirably enhanced. The specific area capacitances and volumetric capacitances of N-doped GF-based EDLC increases 26% and 89% in average, respectively, at different current densities compared with the non-doped GF-based EDLC. In addition, both the energy and power densities are improved, and impressively, the energy densities improve 87% by the N-doping of GF electrodes. The GF-based EDLC also provides the desirable stability that no degradation can be observed within 10,000 cycles. Finally, the flexible N-doped GF-based EDLC is also tested as a wearable supercapacitor, exhibiting no capacitance decrease under the dynamic bending situation. Our approach to synthesize the N-doped GF electrodes can achieve the fine-scale nano-structured GF electrodes and provide a new way forward for improved energy storage devices.