Controllable Construction of Active Sites for Catalytic Conversion and Spatial Constraints Applied to High‐Performance Lithium–Sulfur Batteries

Abstract The structural control of the positive sulfur carrier is very important to inhibit the shuttle effect of polysulfide and improve the overall performance of lithium–sulfur batteries. However, the microstructure of the carbon material carrier is uncontrollable, and it is difficult to coordinate and unify the pores and active sites. Here, Nitrogen and phosphorus co‐doped porous carbon (N/P‐LPC‐900) is obtained through the simple activation method of potassium phosphate to achieve the structural regulation of porous and heteroatoms in one step. N/P‐LPC‐900 shows a graphene‐like porous thin structure, which will provide the particular domain to adsorb polysulfide. The DFT results indicate that N‐6‐P has the strongest catalytic sulfur conversion ability. Further, in situ Raman characterization proves that the signals of Li ₂ S ₆ and Li ₂ S ₄ on the anode side of the N/P‐LPC‐900 battery are significantly weakened after the end of the first stage of discharge. Theory combined with experiment to verify that the co‐doping of N and P for LPC can efficiently catalyze the conversion of polysulfide into Li ₂ S to inhibit the shuttle effect. This work provides a feasible way for the study of sulfur carriers, and lays a theoretical foundation for the construction of high‐performance heteroatom doped porous carbon.