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This content will become publicly available on April 4, 2019

Title: Revealing reaction mechanisms of nanoconfined Li 2 S: implications for lithium–sulfur batteries

Using Li 2S as an active material and designing nanostructured cathode hosts are considered as promising strategies to improve the performance of lithium–sulfur (Li–S) batteries. Here in this study, the reaction mechanisms during the delithiation of nanoconfined Li 2S as an active material, represented by a Li 20S 10 cluster, are examined by first-principles based calculations and analysis. Local reduction and disproportionation reactions can be observed although the overall delithiation process is an oxidation reaction. Long-chain polysulfides can form as intermediate products; however they may bind to insoluble S 2-via Li atoms as mediators. Activating the charging process only requires an overpotential of 0.37 V if using Li 20S 10 as the active material. Sulfur allotropes longer than cyclo-S 8 are observed at the end of the charge process. Although the discharge voltage of Li 20S 10 is only 1.27 V, it can still deliver an appreciable theoretical energy density of 1480 W h kg-1. This study also suggests that hole polarons, in Li 20S 10 and intermediate products, can serve as carriers to facilitate charge transport. This work provides new insights toward revealing the detailed reaction mechanisms of nanoconfined Li 2S as an active material in the Li–S batterymore » cathode.« less
Authors:
 [1] ;  [2] ;  [1] ; ORCiD logo [3] ; ORCiD logo [1] ; ORCiD logo [4] ;  [5]
  1. Hunan Univ., Changsha (China). College of Materials Science and Engineering
  2. Hunan Univ., Changsha (China). College of Materials Science and Engineering, and School of Physics and Electronics
  3. Hunan Univ., Changsha (China). College of Materials Science and Engineering; Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear Engineering and Radiological Science
  4. Texas A & M Univ., College Station, TX (United States)
  5. Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
Publication Date:
Grant/Contract Number:
EE0008210; EE0006832; 51771073; 51772089
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 17; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
Texas A&M Univ., College Station, TX (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium-sulfur battery; density functional theory; charge reactions
OSTI Identifier:
1460762
Alternate Identifier(s):
OSTI ID: 1434225