Defect Engineering of Disordered Carbon Anodes with Ultra-High Heteroatom Doping Through a Supermolecule-Mediated Strategy for Potassium-Ion Hybrid Capacitors

Amorphous carbons are promising anodes for high-rate potassium-ion batteries. Most low-temperature annealed amorphous carbons display unsatisfactory capacities. Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities. Nevertheless, most lignocellulose biomasses lack heteroatoms, making it a challenge to design highly heteroatom-doped carbons (> 10 at%). Herein, we report a new preparation strategy for amorphous carbon anodes. Nitrogen/sulfur co-doped lignin-derived porous carbons (NSLPC) with ultra-high nitrogen doping levels (21.6 at% of N and 0.8 at% of S) from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy. This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product, which induces the formation of high heteroatom doping in the obtained NSLPC. This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K(+) and improved kinetics. The NSLPC anode delivered a high reversible capacity of 419 mAh g(‒1) and superior cycling stability (capacity retention of 96.6% at 1 A g(‒1) for 1000 cycles). Potassium-ion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability (91% capacity retention for 2000 cycles) and a high energy density of 71 Wh kg(–1) at a power density of 92 W kg(–1). [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-01006-0.