Enhanced electrochemical performances of heteroatom-enriched carbon with hierarchical pores prepared by trehalose as a pore-forming agent and a simple one-step carbonization/activation process for supercapacitors

It is highly desired to simultaneously introduce active heteroatoms and abundant hierarchical pore structures for enhanced electrochemical performances on carbon materials. Herein, trehalose as a pore-forming agent was added into polyvinylpyrrolidone/melamine formaldedyde resin mixture with high concentrations of nitrogen and oxygen. Then a simple one-step carbonization/activation process was adopted and heteroatom-enriched carbon with hierarchical pores (HPC) was fabricated successfully. HPC/HPC symmetric supercapacitors were assembled using KOH electrolyte. It is clearly demonstrated that due to the pore-forming action of trehalose HPC shows the porous honeycomb, interconnected and worm-like pore structure, which is favorable to enhance the double-layer capacitance. It is confirmed that in our system the three active species of pyridinic nitrogen (N-6), pyrrolic nitrogen (N-5) and quinone type oxygen (O-I) are responsible for the pseudocapacitive behavior. Based on XPS, nitrogen adsorption/desorption isotherms and electrochemical impedance spectroscopy, it is deduced that the ratio-optimized HPC-T30 exhibits high concentration of three active species (8.17 at.%), increased specific area (351.26 m² g⁻¹) and tuned hierarchical pore structures with substantial micropores (micropore area of 321.68 m² g⁻¹) and a small amount of mesopores and macropores, which lead to decrease of charge transfer resistance, increase of transfer rate of electrolyte ions in the pores and excellent electrochemical performances. In cyclic voltammetry tests of three-electrode system and galvanostatic charge/discharge tests of two-electrode system, HPC-T30 displays high specific capacitance, 46% and 1.2-time enhancement compared to untreated HPC-T0, respectively. The optimized HPC-T30/HPC-T30 supercapacitor delivers the energy density of 6.69 W h kg⁻¹ in 6 M KOH electrolyte. Furthermore, the supercapacitor shows a capacitance retention of 91.16% up to 6000 cycles and the coulombic efficiency reaches nearly 100% for each charged/discharge cycle, demonstrating its good cyclic stability.