Insight into a Nitrogen-Doping Mechanism in a Hard-Carbon-Microsphere Anode Material for the Long-Term Cycling of...

To investigate the alternatives to lithium-ion batteries, potassium-ion batteries have attracted considerable interest due to the cost-efficiency of potassium resources and the relatively lower standard redox potential of K⁺/K. Among various alternative anode materials, hard carbon has the advantages of extensive resources, low cost, and environmental protection. In the present study, we synthesize a nitrogen-doping hard-carbon-microsphere (N-SHC) material as an anode for potassium-ion batteries. N-SHC delivers a high reversible capacity of 248 mAh g^-1 and a promoted rate performance (93 mAh g^-1 at 2 A g^-1). Additionally, the nitrogen-doping N-SHC material also exhibits superior cycling long-term stability, where the N-SHC electrode maintains a high reversible capacity at 200 mAh g^-1 with a capacity retention of 81% after 600 cycles. DFT calculations assess the change in K ions' absorption energy and diffusion barriers at different N-doping effects. Compared with an original hard-carbon material, pyridinic-N and pyrrolic-N defects introduced by N-doping display a positive effect on both K ions' absorption and diffusion.