A reversible
lithium-sulfur battery is considered one of the most
promising high-energy-density energy storage systems. Organic sulfide
cathodes have attracted widespread attention due to their flexibility
and diversity. N doping is one of the methods to improve the performance
of organic sulfide cathodes. Py2S
n
(2 ≤ n ≤ 8), as a kind of N-containing
molecule, has shown high specific capacity and good cycle performance
in the experiment. Here, we will reveal the mechanism of its excellent
electrochemical performance by density functional theory. In the process
of charging and discharging, the formation of a Li bond (N–Li)
increases the specific capacity of the battery, and the products with
the lithium bond can adsorb polysulfides to inhibit the shuttle effect,
which is very important for resisting capacity degradation and improving
cycle stability. This work also confirms the importance of Li-bond
chemistry in the design of organic sulfide cathode materials, which
will help provide different thoughts and ideas for future cathode
material design.