Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 3, Issue 32, Pages 16670-16678Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5ta04255k
Keywords
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Funding
- ARC Discovery Grants from Australian Research Council
- NSFC-RGC Joint Research Scheme [51361165201]
- NSFC [51125001, 51172005]
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Conductive confinement of sulfur and polysulfides via carbonaceous blocking layers can simultaneously address the issues of low conductivity, volume expansion of sulfur during the charge/discharge process and the polysulfide shuttling effect in lithium-sulfur (Li-S) batteries. Herein, a conductive and porous nitrogen and phosphorus dual doped graphene (p-NP-G) blocking layer is prepared via a thermal annealing and subsequent hydrothermal reaction route. The doping levels of N and P in p-NP-G as measured by X-ray photoelectron spectroscopy are ca. 4.38% and ca. 1.93%, respectively. The dual doped blocking layer exhibits higher conductivity than N or P single doped blocking layers. More importantly, density functional theory (DFT) calculations demonstrate that P atoms and -P-O groups in the p-NP-G layer offer stronger adsorption of polysulfides than the N species. The electrochemical evaluation results illustrate that the p-NP-G blocking layer can deliver superior initial capacity (1158.3 mA h g(-1) at a current density of 1C), excellent rate capability (633.7 mA h g-1 at 2C), and satisfactory cycling stability (ca. 0.09% capacity decay per cycle), which are better than those of the N or P single doped graphene. This work suggests that this synergetic combination of conductive and adsorptive confinement strategies induced by the multi-heteroatom doping scheme is a promising approach for developing high performance Li-S batteries.
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