Nitrogen‐Doped Carbon and Metal‐Nitrogen–Carbon Materials as Cathode Hosts for Li–S Batteries: Experimental Study and Mechanism Analysis

Both nitrogen‐doped carbon (NC) and metal‐nitrogen‐carbon (MNC) materials have been extensively investigated in lithium‐sulfur batteries to alleviate the “shuttle effect”. MNC are generally synthesized using NC as the parent material, wherein nitrogen atoms in NC serve as the “bridge” to coordinate with metal atoms. So far, an important scientific issue has not been settled: does the introduction of metal sites into NC certainly enhance the Li–S battery performance? In this work, NC and MNC materials derived from the same precursor, a nitrogen‐rich porous polymer, are systematically compared as cathode hosts for Li–S battery through theoretical calculations and experimental investigation. Li–S cell with NC as the cathode sulfur host exhibits better cycle performance at low current densities (0.1 and 0.2C), whereas MNC materials predominate at higher current densities (such as 1C and 2C). Based on theoretical calculation and experimental results, it is concluded that the introduction of metal sites into NC through nitrogen bonding promoted the catalytic capability for faster sulfur redox reaction kinetics, whereas the adsorption energy toward polysulfides decreased. This work provides important guidance for more targeted design of advanced materials for lithium–sulfur battery application in the future. Nitrogen‐doped carbon (NC) and metal‐nitrogen‐carbon (MNC) materials have their own pros and cons for Li–S battery application: NC possesses higher adsorption energies toward polysulfides, while MNC materials are more efficient in accelerating sulfur redox reaction kinetics. As a result, NC enables better performance than MNC materials at low current densities, whereas MNC materials predominate at high current densities.