Lithium-sulfur (Li-S) batteries are promising energy storage systems due to their large theoretical energy density of 2600 Wh kg −1 and cost effectiveness. However, the severe shuttle effect of soluble lithium polysulfide intermediates (LiPSs) and sluggish redox kinetics during the cycling process cause low sulfur utilization, rapid capacity fading, and a low coulombic efficiency. Here, a 3D copper, nitrogen co-doped hierarchically porous graphitic carbon network developed through a freeze-drying method (denoted as 3D Cu@ NC-F) is prepared, and it possesses strong chemical absorption and electrocatalytic conversion activity for LiPSs as highly efficient sulfur host materials in Li-S batteries. The porous carbon network consisting of 2D cross-linked ultrathin carbon nanosheets provides void space to accommodate volumetric expansion upon lithiation, while the Cu, N-doping effect plays a critical role for the confinement of polysulfides through chemical bonding. In addition, after sulfuration of Cu@NC-F network, the in situ grown copper sulfide (Cu x S) embedded within Cu x S@NC/S-F composite catalyzes LiPSs conversion during reversible cycling, resulting in low polarization and fast redox reaction kinetics. At a current density of 0.1 C, the Cu x S@NC/S-F composites' electrode exhibits an initial capacity of 1432 mAh g −1 and maintains 1169 mAh g −1 after 120 cycles, with a coulombic efficiency of nearly 100%. development of advanced energy storage systems. Li-S batteries have been considered a new generation energy storage system because of their high theoretical energy density of 2600 Wh kg −1 and theoretical specific capacity of 1675 mAh g −1 , [1] and the merits of safe, low-cost and nonpolluting also make these batteries an exceptional storage system. To date, researchers' knowledge of boosting the energy density of Li-S batteries has resulted in an increase in energy density to 500 Wh kg −1 or more. However, a series of problems inherent in Li-S batteries remain unsolved, such as the low conductivity of sulfur (5 × 10 −30 S cm −1 at 25 °C) and its discharge products (Li 2 S/Li 2 S 2 ), [2] the solubility and shuttle effect of long-chain LiPS intermediates (Li 2 S n , 4 ≤ n ≤ 8), and large volume expansion of ≈80% cause low sulfur utilization, rapid capacity fading, and poor rate-performance and low coulombic efficiency, which still limit practical applications of Li-S batteries. [3,4] At the current stage of Li-S battery research, research has been concentrated on reducing the shuttle effect by advancing electrolyte additives, [5] optimizing cathode structures, [6] using modified separators or bifunctional interlayers, [7,8] and devising protective anode structures, [9] to enable sufficient protection and
Lithium-Sulfur BatteriesThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.