electrochemical energy storage devices due to the natural abundance of elemental sulfur, low cost, high theoretical specific capacity (1675 mAh g −1 ), and energy density (2600 Wh kg −1 ). [1][2][3] Despite these tempting properties, their practical applications are still plagued by several serious obstacles, such as incomplete utilization of insulating sulfur, troublesome shuttling effect of soluble polysulfides (Li 2 S n , 4 ≤ n ≤ 8), and large volume expansion of sulfur (≈80%), resulting in low practical energy density and rapid capacity fading during the battery cycling. [4,5] With the purpose of overcoming these issues, numerous efforts have been dedicated to improving the electrochemical performance of Li-S batteries by some typical strategies, such as physical confinement and chemical binding of sulfur species into diverse host materials (e.g., hollow carbon nanomaterials, [6,7] metallic compounds, [8][9][10][11] ) separator/interlayer design, [12][13][14] multifunctional polar binders, [15,16] electrolyte modification, [17,18] and lithium anode protection. [19,20] Although these sulfur-hosting composites have been proved to efficiently inhibit polysulfides shuttling between the cathode and the lithium anode, their low sulfur content in cathode leads to their energy density cutting in half at most compared with the pure sulfur/carbon black (CB) cathode Lithium-sulfur (Li-S) batteries have been disclosed as one of the most promising energy storage systems. However, the low utilization of sulfur, the detrimental shuttling behavior of polysulfides, and the sluggish kinetics in electrochemical processes, severely impede their application. Herein, 3D hierarchical nitrogen-doped carbon nanosheets/molybdenum phosphide nanocrystal hollow nanospheres (MoP@C/N HCSs) are introduced to Li-S batteries via decorating commercial separators to inhibit polysulfides diffusion. It acts not only as a polysulfides immobilizer to provide strong physical trapping and chemical anchoring toward polysulfides, but also as an electrocatalyst to accelerate the kinetics of the polysulfides redox reaction, and to lower the Li 2 S nucleation/dissolution interfacial energy barrier and selfdischarge capacity loss in working Li-S batteries, simultaneously. As a result, the Li-S batteries with MoP@C/N HCS-modified separators show superior rate capability (920 mAh g −1 at 2 C) and stable cycling life with only 0.04% capacity decay per cycle over 500 cycles at 1 C with nearly 100% Coulombic efficiency. Furthermore, the Li-S battery can achieve a high area capacity of 5.1 mAh cm −2 with satisfied capacity retention when the cathode loading reaches 5.5 mg cm −2 . This work offers a brand new guidance for rational separator design into the energy chemistry of high-stable Li-S batteries.
Lithium-Sulfur BatteriesThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.