Abstract

Lithium–sulfur batteries are regarded as very promising energy storage devices due to their high energy density, low cost, and environmental friendliness; however, their insulating properties and the instability of sulfur‐based electrodes impede the practical applications of Li–S batteries. Here, a versatile strategy to synthesize double‐shelled nitrogen and phosphorus codoped carbon spheres (NPDSCS) as an efficient sulfur host for Li–S batteries is reported. With strong trapping, good affinity, high adsorption for polysulfides, and the bifunctional catalyzing for sulfur redox processes, the developed NPDSCS cathodes with a high S loading of 72.4% exhibit large specific discharge capacity of 1326 mAh g−1 at 0.1C, high Coulombic efficiency, good rate capability, and excellent cycling performance with a reversible capacity of 814 mAh g−1 at 1C after 500 cycles.

Highlights

  • Good affinity, high adsorption for polysulfides, and the bifunctional catalyzing for sulfur redox processes, the developed NPDSCS cathodes with a high S loading of 72.4% exhibit large specific discharge capacity of 1326 mAh g−1 at 0.1C, high Coulombic advantages endow their great potential to power electric vehicles and intensive renewable energy storage, which require power sources with high energy and power density as well as long cycle life

  • We demonstrate for the first time that double-shelled hollow carbon spheres (HCSs) with controllable structures can be directly templating synthesized using double-shelled SiO2 hollow capsules, which are precisely controlled by selectively etching solid silica@mesoporous silica nanospheres in a mildly alkaline solution

  • Good affinity, high adsorption for polysulfides, and the bifunctional catalyzing for sulfur redox processes, this NPDSCS has been demonstrated an efficient matrix for sulfur

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Summary

Synthesis and Characterization of NPDSCS-S Composites

The dark area part in the core and shell of NPDSCS can be assigned to sulfur, which shows the opposite contrast in the STEM image (Figure 2e). NPDSCS exhibits a high surface area of 1285.6 m2 g−1 and a large pore volume of 1.91 cm g−1. Surprisingly, the Brunauer–Emmett–Teller (BET) specific surface area of NPDSCS-S decreases to 19.3 m2 g−1 and the pore volume drops to 0.24 cm g−1, indicating the successful impregnation of sulfur into NPDSCS. The high-resolution P 2p spectrum in Figure 4d can be deconvoluted into 2p 3/2 and 2p 1/2 peaks centered at 132.5 and 134 eV, which can be attributed to the interactions of P C and P O, respectively.[50]

The Electrochemical Performance of NPDSCS-S Cathodes
Conclusion
Experimental Section
Conflict of Interest
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