A Multidimensional Operando Study Showing the Importance of the Electrode Macrostructure in Lithium Sulfur Batteries
Abstract
Lithium sulfur batteries are one of the most promising next-generation energy storage technologies, because of their impressive theoretical energy density, low materials cost, and relative safety. However, incomplete understanding of their underlying operation mechanisms has hindered their further development and commercialization. In this work, to gain a better understanding of the operation mechanisms in the lithium sulfur battery, three macroscopically different (woven and nonwoven) and microscopically similar (made from the same carbon fibers) free-standing carbon felts are used as the conductive matrices to show how the macrostructure influences the redox reactions and the electrochemical performance. Additionally, an operando radiography and simultaneous in situ electrochemical impedance spectroscopy study are performed to highlight the differences of the carbon hosts and how they compare electrochemically in a lithium sulfur battery. The electrochemical results show that the carbon host with a more open structure results in increased capacity as well as a higher diffusion coefficient. The operando radiography shows that the open structures are more conducive to efficient redox reactivity in forming solid sulfur species, mostly in the form of elongated needlelike structures identified as β-S8, near the end of charge, which is corroborated by the impedance data. The data also reveal a “breathing”more »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Institute of Applied Materials, Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin (Germany)
- Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin (Germany)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES), Materials Sciences and Engineering Division
- OSTI Identifier:
- 1649254
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Energy Materials
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2574-0962
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Redox reactions; sulfur; carbon fiber; chemical structure; batteries; lithium polysulfide batteries; macrostructure; radiography; EIS; breathing mechanism
Citation Formats
Jafta, Charl J., Hilger, André, Sun, Xiao-Guang, Geng, Linxiao, Li, Mengya, Risse, Sebastian, Belharouak, Ilias, and Manke, Ingo. A Multidimensional Operando Study Showing the Importance of the Electrode Macrostructure in Lithium Sulfur Batteries. United States: N. p., 2020.
Web. doi:10.1021/acsaem.0c01027.
Jafta, Charl J., Hilger, André, Sun, Xiao-Guang, Geng, Linxiao, Li, Mengya, Risse, Sebastian, Belharouak, Ilias, & Manke, Ingo. A Multidimensional Operando Study Showing the Importance of the Electrode Macrostructure in Lithium Sulfur Batteries. United States. https://doi.org/10.1021/acsaem.0c01027
Jafta, Charl J., Hilger, André, Sun, Xiao-Guang, Geng, Linxiao, Li, Mengya, Risse, Sebastian, Belharouak, Ilias, and Manke, Ingo. Tue .
"A Multidimensional Operando Study Showing the Importance of the Electrode Macrostructure in Lithium Sulfur Batteries". United States. https://doi.org/10.1021/acsaem.0c01027. https://www.osti.gov/servlets/purl/1649254.
@article{osti_1649254,
title = {A Multidimensional Operando Study Showing the Importance of the Electrode Macrostructure in Lithium Sulfur Batteries},
author = {Jafta, Charl J. and Hilger, André and Sun, Xiao-Guang and Geng, Linxiao and Li, Mengya and Risse, Sebastian and Belharouak, Ilias and Manke, Ingo},
abstractNote = {Lithium sulfur batteries are one of the most promising next-generation energy storage technologies, because of their impressive theoretical energy density, low materials cost, and relative safety. However, incomplete understanding of their underlying operation mechanisms has hindered their further development and commercialization. In this work, to gain a better understanding of the operation mechanisms in the lithium sulfur battery, three macroscopically different (woven and nonwoven) and microscopically similar (made from the same carbon fibers) free-standing carbon felts are used as the conductive matrices to show how the macrostructure influences the redox reactions and the electrochemical performance. Additionally, an operando radiography and simultaneous in situ electrochemical impedance spectroscopy study are performed to highlight the differences of the carbon hosts and how they compare electrochemically in a lithium sulfur battery. The electrochemical results show that the carbon host with a more open structure results in increased capacity as well as a higher diffusion coefficient. The operando radiography shows that the open structures are more conducive to efficient redox reactivity in forming solid sulfur species, mostly in the form of elongated needlelike structures identified as β-S8, near the end of charge, which is corroborated by the impedance data. The data also reveal a “breathing” mechanism, where the polysulfides are pushed to the edges during discharge and pulled back during charge. Furthermore, it is also revealed that the “breathing” process is a limiting factor in the high rate performance. Overall, this study shows that there is a close relationship between the macrostructure of the carbon matrix and the electrochemical performance of the sulfur cathode.},
doi = {10.1021/acsaem.0c01027},
journal = {ACS Applied Energy Materials},
number = 7,
volume = 3,
place = {United States},
year = {Tue Jun 23 00:00:00 EDT 2020},
month = {Tue Jun 23 00:00:00 EDT 2020}
}
Web of Science
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