Free-Standing Nitrogen-doped Graphene Paper as Electrodes for High-Performance Lithium/Dissolved Polysulfide Batteries

Kai Han, Jingmei Shen, Shiqiang Hao, Hongqi Ye, Christopher Wolverton, Mayfair C. Kung, Harold H Kung

Research output: Contribution to journalArticle

95 Citations (Scopus)

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 approximately1000 mA h g−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 DFT calculation, 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.

Original languageEnglish
Pages (from-to)2545-2553
Number of pages9
JournalChemSusChem
Volume7
Issue number9
DOIs
Publication statusPublished - 2014

Fingerprint

Polysulfides
Graphite
lithium
Lithium
Graphene
electrode
Nitrogen
Electrodes
nitrogen
electron microscopy
electrolyte
pyrolysis
X-ray spectroscopy
spectroscopy
X-ray diffraction
chloride
sulfide
Atoms
modeling
Sulfides

Keywords

  • binder-free
  • catholyte
  • free-standing
  • Li/polysulfide battery
  • N-doped graphene

ASJC Scopus subject areas

  • Environmental Chemistry
  • Chemical Engineering(all)
  • Materials Science(all)
  • Energy(all)

Cite this

Free-Standing Nitrogen-doped Graphene Paper as Electrodes for High-Performance Lithium/Dissolved Polysulfide Batteries. / Han, Kai; Shen, Jingmei; Hao, Shiqiang; Ye, Hongqi; Wolverton, Christopher; Kung, Mayfair C.; Kung, Harold H.

In: ChemSusChem, Vol. 7, No. 9, 2014, p. 2545-2553.

Research output: Contribution to journalArticle

Han, Kai ; Shen, Jingmei ; Hao, Shiqiang ; Ye, Hongqi ; Wolverton, Christopher ; Kung, Mayfair C. ; Kung, Harold H. / Free-Standing Nitrogen-doped Graphene Paper as Electrodes for High-Performance Lithium/Dissolved Polysulfide Batteries. In: ChemSusChem. 2014 ; Vol. 7, No. 9. pp. 2545-2553.
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