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- Title
Free-Standing Nitrogen-doped Graphene Paper as Electrodes for High-Performance Lithium/Dissolved Polysulfide Batteries.
- Authors
Han, Kai; Shen, Jingmei; Hao, Shiqiang; Ye, Hongqi; Wolverton, Christopher; Kung, Mayfair C.; Kung, Harold H.
- Abstract
Free-standing N-doped graphene papers (NGP), generated by pyrolysis of polydiallyldimethylammonium chloride, were successfully used as binder-free electrodes for the state-of-the-art Li/polysulfide-catholyte batteries. They exhibited high specific capacities of approximately 1000 mAhg-1 (based on S) after 100 cycles and coulombic efficiencies great than 98%, significantly better than undoped graphene paper (GP). These NGP were characterized with XRD, X-ray photoelectron spectroscopy, thermogravimetric analysis, AFM, electron microscopy, and Raman and impedance spectroscopy before and after cycling. Spectroscopic evidence suggested stronger binding of sulfide to NGP relative to GP, and modelling results from DFTcalculation, substantiated with experimental data, indicated that pyrrolic and pyridinic N atoms interacted more strongly with Li polysulfides than quaternary N atoms. Thus, more favorable partition of polysulfides between the electrode and the electrolyte and the corresponding effect on the morphology of the passivation layer were the causes of the beneficial effect of N doping.
- Subjects
PYROLYSIS; GRAPHENE; ELECTRODES; LITHIUM cells; ELECTRIC batteries research
- Publication
ChemSusChem, 2014, Vol 7, Issue 9, p2545
- ISSN
1864-5631
- Publication type
Article
- DOI
10.1002/cssc.201402329