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Title: Nucleophilic substitution between polysulfides and binders unexpectedly stabilizing lithium sulfur battery

Polysulfide shuttling has been the primary cause of failure in lithium-sulfur (Li-S) battery cycling. In this paper, we demonstrate an nucleophilic substitution reaction between polysulfides and binder functional groups can unexpectedly immobilizes the polysulfides. The substitution reaction is verified by UV–visible spectra and X-ray photoelectron spectra. The immobilization of polysulfide is in situ monitored by synchrotron based sulfur K-edge X-ray absorption spectra. The resulting electrodes exhibit initial capacity up to 20.4 mAh/cm 2, corresponding to 1199.1 mAh/g based on a micron-sulfur mass loading of 17.0 mg/cm 2. The micron size sulfur transformed into nano layer coating on the cathode binder during cycling. Directly usage of nano-size sulfur promotes higher capacity of 33.7 mAh/cm 2, which is the highest areal capacity reported in Li-S battery. Finally, this enhance performance is due to the reduced shuttle effect by covalently binding of the polysulfide with the polymer binder.
 [1] ;  [2] ;  [1] ;  [2] ;  [2] ;  [3] ;  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Applied Energy Materials Group. Energy Storage and Distributed Resources Division
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  3. Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing
Publication Date:
Grant/Contract Number:
AC02-05CH11231; 2016YFA0202603; 51425204
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 38; Journal ID: ISSN 2211-2855
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Wuhan Univ. of Technology (China)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Key Research and Development Program of China; National Natural Science Fund for Distinguished Young Scholars (China)
Country of Publication:
United States
25 ENERGY STORAGE; nucleophilic substitution; poly(vinyl sulfate); carrageenan; chemical binding; high loading electrodes; lithium sulfur battery
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1396405