Nitrogen-rich accordion-like lignin porous carbon via confined self-assembly template and in-situ mild activation strategy for high-performance supercapacitors

Abstract

Nitrogen-doped porous carbons have emerged as promising electrode materials for supercapacitors. However, the precise control of carbon geometry and the effective doping method remain challenging. Herein, a confined self-assembly template and in-situ mild activation strategy is proposed to prepare cubic lignin composite precursor, followed by co-pyrolysis with melamine at a high temperature for nitrogen-doped hierarchical porous carbons (N-HPLCs). The zinc oxalate template has the coupling effect of confinement and mild activation during carbonization, which not only prevents the restacking of the carbon matrix but also generates zinc cyanamide intermediate to avoid excessive loss of nitrogen species. The optimized N-HPLCs exhibit an accordion-like framework with interconnected porous sheets, ultrahigh edge-nitrogen doping level (up to 12.20 at.%), and a total nitrogen doping level of 14.09 at.%. Consequently, it shows a high gravimetric capacitance of 354 F/g at 0.2 A/g, an extraordinary surface-area-normalized capacitance of 82.1 ± 0.2 μF/cm2, and good rate capability in supercapacitor applications. Moreover, the fabricated coin-type symmetric supercapacitor displays a high energy density of 12.9 Wh/kg at 161.9 W/kg and superior cycling stability with a 99.5% capacitance retention after 16,000 cycles at 2.0 A/g. This work offers a novel method for preparing nitrogen-enriched lignin-derived carbon for high-performance supercapacitors.