Journal
ADVANCED ENERGY MATERIALS
Volume 10, Issue 20, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202000651
Keywords
electrocatalytic effects; lithium-sulfur batteries; metal sulfides; porous carbon spheres; pyrrhotite
Categories
Funding
- Dalian National Laboratory for Clean Energy (DNL), CAS
- DNL Cooperation Fund, CAS [DNL180402, DNL180310, DNL180308, DNL201912, DNL201915]
- Engineering and Physical Sciences Research Council [EP/R021554/1]
- National Key R&D Program of China [2016YBF0100100]
- National Natural Science Foundation of China [51872283, 21805273]
- Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science [20180510038]
- Liaoning Revitalization Talents Program [XLYC1807077, XLYC1807153]
- DICP [DICP ZZBS201708, DICP ZZBS201802]
- DICPQIBEBT [DICP UN201702, QIBEBT UN201702]
- EPSRC [EP/P020232/1, EP/P020194/1]
- Eureka HPC cluster at the University of Surrey
- Natural Science Foundation of Liaoning Province
- EPSRC [EP/P020232/1, EP/R021554/1, EP/R021554/2, EP/P020194/1] Funding Source: UKRI
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Lithium-sulfur batteries (LSBs) are a class of new-generation rechargeable high-energy-density batteries. However, the persisting issue of lithium polysulfides (LiPs) dissolution and the shuttling effect that impedes the efficiency of LSBs are challenging to resolve. Herein a general synthesis of highly dispersed pyrrhotite Fe1-xS nanoparticles embedded in hierarchically porous nitrogen-doped carbon spheres (Fe1-xS-NC) is proposed. Fe1-xS-NC has a high specific surface area (627 m(2) g(-1)), large pore volume (0.41 cm(3) g(-1)), and enhanced adsorption and electrocatalytic transition toward LiPs. Furthermore, in situ generated large mesoporous pores within carbon spheres can accommodate high sulfur loading of up to 75%, and sustain volume variations during charge/discharge cycles as well as improve ionic/mass transfer. The exceptional adsorption properties of Fe1-xS-NC for LiPs are predicted theoretically and confirmed experimentally. Subsequently, the electrocatalytic activity of Fe1-xS-NC is thoroughly verified. The results confirm Fe1-xS-NC is a highly efficient nanoreactor for sulfur loading. Consequently, the Fe1-xS-NC nanoreactor performs extremely well as a cathodic material for LSBs, exhibiting a high initial capacity of 1070 mAh g(-1) with nearly no capacity loss after 200 cycles at 0.5 C. Furthermore, the resulting LSBs display remarkably enhanced rate capability and cyclability even at a high sulfur loading of 8.14 mg cm(-2).
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