Rational Construction of Fe2N@C Yolk–Shell Nanoboxes as Multifunctional Hosts for Ultralong Lithium–Sulfur Batteries

Rationally constructing inexpensive sulfur hosts that have high electronic conductivity, large void space for sulfur, strong chemisorption, and rapid redox kinetics to polysulfides is critically important for their practical use in lithium–sulfur (Li–S) batteries. Herein, we have designed a multifunctional sulfur host based on yolk–shelled Fe 2 N@C nanoboxes (Fe 2 N@C NBs) through a strategy of etching combined with nitridation for high-rate and ultralong Li–S batteries. The highly conductive carbon shell physically confines the active material and provides efficient pathways for fast electron/ion transport. Meanwhile, the polar Fe 2 N core provides strong chemical bonding and effective catalytic activity for polysulfides, which is proved by density functional theory calculations and electrochemical analysis techniques. Benefiting from these merits, the S/Fe 2 N@C NBs electrode with a high sulfur content manifests a high specific capacity, superior rate capability, and long-term cycling stability. Specifically, even after 600 cycles at 1 C, a capacity of 881 mAh g –1 with an average fading rate of only 0.036% can be retained, which is among the best cycling performances reported. The strategy in this study provides an approach to the design and construction of yolk–shelled iron-based compounds@carbon nanoarchitectures as inexpensive and efficient sulfur hosts for realizing practically usable Li–S batteries.