Pseudocapacitive Contribution in Sulfur-Doped Porous Carbon Nanosheets Enables High-Performance Sodium-Ion Storage

Sulfur-doped carbon materials have sparked considerable attention as the anodes for sodium-ion batteries (SIBs) due to their relatively high reversible specific capacity and excellent pseudocapacitive effect. However, the content of sulfur dopants in carbon materials is usually limited and an efficient doping strategy is urgently imperative to date. Herein, a space-confined doping strategy is proposed to fabricate porous carbon nanosheets with high sulfur dopant content by using low-cost pitch as a precursor with the help of sodium thiosulfate (Na2S2O3). The thermostable nano-MgO used in this system can occupy the specific space during pitch decomposition to induce the formation of hierarchical carbon nanosheets. Interestingly, such a space-confinement effect of nano-MgO is able to enlarge the accessible contact area of reactants and inhibit the loss of sulfur from Na2S2O3, thus significantly increasing sulfur dopant content within carbon frameworks. The optimized sulfur-doped carbon nanosheets (S-PCNs-2) with a high sulfur content of about 20.56 wt.% as anode for SIBs delivers an ultrahigh pseudocapacitive contribution of 92.55% at 5 mV s-1 and thus enable a desirable specific capacity of 428.6 mAh g-1 at 0.1 A g-1 with a high initial Coulombic efficiency of 84.9% and superior rate performance of 380.6 mAh g-1 at 5 A g-1. Furthermore, a long cycling lifespan with a capacity retention of 88% after 1000 charge/discharge cycles can be achieved for the S-PCNs-2 anode. This work provides a simple yet efficient doping approach to fabricate carbon anodes with high heteroatom contents for SIBs.