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Title: Synthesis and Characterization of a Molecularly Designed High-Performance Organodisulfide as Cathode Material for Lithium Batteries

Abstract

An innovative organodisulfide compound, 2,3,4,6,8,9,10,12–Octathia biscyclopenta[b,c]–5,11–anthraquinone–1,7–dithione (TPQD), has been successfully designed, synthesized, and characterized as a cathode material for lithium batteries. A benzoquinone is introduced to coordinate with dithiolane through 1,4–dithianes. The molecular structure, electrochemical performances, and the lithiation/delithiation mechanism of the TPQD cathode have been systematically investigated. TPQD can deliver an initial capacity of 251.7 mAh g-1 at a rate of C/10, which corresponds to the transfer of 4.7 electrons per formula. Highly reversible capacities and stable cyclic performances can be achieved at rates from C/10 to 5 C. Very interestingly, TPQD can retain a capacity of 120 mAh g-1 after 200 cycles at the 5 C rate, which is quite impressive for organodisulfide compounds. X–ray absorption spectroscopy measurements and density functional theory calculation results suggest that such a high capacity is contributed by both O redox of the quinone group and the cleavage and recombination of the disulfide bond. Moreover, the extended π–conjugation structure of the material, introduced by benzoquinone and dithiane, is beneficial for improving the high rate capability and cyclic stability. Furthermore this study illustrates an innovative approach in designing new organodisulfide compounds with improved cyclability and rate capability as cathode materials for high performance lithiummore » batteries.« less

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [3];  [3];  [3];  [4];  [1]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Jingdezhen Ceramic Institute, Jingdezhen (China)
  3. Canadian Light Source, Saskatoon (Canada)
  4. Stony Brook Univ., Stony Brook, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1507114
Alternate Identifier(s):
OSTI ID: 1506702
Report Number(s):
BNL-211534-2019-JAAM
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 21; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; organodisulfide; lithium battery; high rate; soft X ray absorption spectroscopy

Citation Formats

Shadike, Zulipiya, Lee, Hung ‐Sui, Tian, Chuanjin, Sun, Ke, Song, Liang, Hu, Enyuan, Waluyo, Iradwikanari, Hunt, Adrian, Ghose, Sanjit, Hu, Yongfeng, Zhou, Jigang, Wang, Jian, Northrup, Paul, Bak, Seong ‐Min, and Yang, Xiao ‐Qing. Synthesis and Characterization of a Molecularly Designed High-Performance Organodisulfide as Cathode Material for Lithium Batteries. United States: N. p., 2019. Web. doi:10.1002/aenm.201900705.
Shadike, Zulipiya, Lee, Hung ‐Sui, Tian, Chuanjin, Sun, Ke, Song, Liang, Hu, Enyuan, Waluyo, Iradwikanari, Hunt, Adrian, Ghose, Sanjit, Hu, Yongfeng, Zhou, Jigang, Wang, Jian, Northrup, Paul, Bak, Seong ‐Min, & Yang, Xiao ‐Qing. Synthesis and Characterization of a Molecularly Designed High-Performance Organodisulfide as Cathode Material for Lithium Batteries. United States. doi:10.1002/aenm.201900705.
Shadike, Zulipiya, Lee, Hung ‐Sui, Tian, Chuanjin, Sun, Ke, Song, Liang, Hu, Enyuan, Waluyo, Iradwikanari, Hunt, Adrian, Ghose, Sanjit, Hu, Yongfeng, Zhou, Jigang, Wang, Jian, Northrup, Paul, Bak, Seong ‐Min, and Yang, Xiao ‐Qing. Wed . "Synthesis and Characterization of a Molecularly Designed High-Performance Organodisulfide as Cathode Material for Lithium Batteries". United States. doi:10.1002/aenm.201900705. https://www.osti.gov/servlets/purl/1507114.
@article{osti_1507114,
title = {Synthesis and Characterization of a Molecularly Designed High-Performance Organodisulfide as Cathode Material for Lithium Batteries},
author = {Shadike, Zulipiya and Lee, Hung ‐Sui and Tian, Chuanjin and Sun, Ke and Song, Liang and Hu, Enyuan and Waluyo, Iradwikanari and Hunt, Adrian and Ghose, Sanjit and Hu, Yongfeng and Zhou, Jigang and Wang, Jian and Northrup, Paul and Bak, Seong ‐Min and Yang, Xiao ‐Qing},
abstractNote = {An innovative organodisulfide compound, 2,3,4,6,8,9,10,12–Octathia biscyclopenta[b,c]–5,11–anthraquinone–1,7–dithione (TPQD), has been successfully designed, synthesized, and characterized as a cathode material for lithium batteries. A benzoquinone is introduced to coordinate with dithiolane through 1,4–dithianes. The molecular structure, electrochemical performances, and the lithiation/delithiation mechanism of the TPQD cathode have been systematically investigated. TPQD can deliver an initial capacity of 251.7 mAh g-1 at a rate of C/10, which corresponds to the transfer of 4.7 electrons per formula. Highly reversible capacities and stable cyclic performances can be achieved at rates from C/10 to 5 C. Very interestingly, TPQD can retain a capacity of 120 mAh g-1 after 200 cycles at the 5 C rate, which is quite impressive for organodisulfide compounds. X–ray absorption spectroscopy measurements and density functional theory calculation results suggest that such a high capacity is contributed by both O redox of the quinone group and the cleavage and recombination of the disulfide bond. Moreover, the extended π–conjugation structure of the material, introduced by benzoquinone and dithiane, is beneficial for improving the high rate capability and cyclic stability. Furthermore this study illustrates an innovative approach in designing new organodisulfide compounds with improved cyclability and rate capability as cathode materials for high performance lithium batteries.},
doi = {10.1002/aenm.201900705},
journal = {Advanced Energy Materials},
number = 21,
volume = 9,
place = {United States},
year = {2019},
month = {4}
}

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