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Title: A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries

Abstract

Lithium–sulfur (Li–S) batteries hold great promise as a next-generation energy-storage technology. Their practical application, however, is hindered by the rapid capacity fading associated with the dissolution of lithium polysulfides (LiPSs) into organic electrolytes. In this work, we successfully impede these losses by anchoring thiol (–SH) functional groups to the nonpolar surface of a mesoporous carbon host. This new strategy increases the surface polarity of conductive carbons and traps LiPSs inside cathodes. By utilizing various spectroscopic methods, we investigate the mechanisms of LiPS trapping, which originate from the electrostatic and covalent interactions of the thiol functional groups with Li+ from the electrolyte and with S from the LiPS chains, respectively. Here, we for the first time identify the multiple interactions that are induced by a small molecular interface upon cycling and correlate them with the electrochemical behavior. The fundamental insight on the thiol functionality suggests a further rational design of multifunctional interfaces to achieve better Li–S performance.

Authors:
 [1];  [2]; ORCiD logo [3];  [2];  [4];  [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [3];  [2];  [1]
  1. UNIVERSITY OF WASHINGTON
  2. University of Washington
  3. BATTELLE (PACIFIC NW LAB)
  4. University of Pittsburgh
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1544787
Report Number(s):
PNNL-SA-144283
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Materials Chemistry A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 21
Country of Publication:
United States
Language:
English

Citation Formats

Li, Yun, Murphy, Ian A., Chen, Ying, Li, Francis, Wang, Xiang, Wang, Shanyu, Hubble, Dion, Jang, Sei-Hum, Mueller, Karl T., Wang, Chongmin, Jen, Alex K.-Y., and Yang, Jihui. A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries. United States: N. p., 2019. Web. doi:10.1039/c9ta02743b.
Li, Yun, Murphy, Ian A., Chen, Ying, Li, Francis, Wang, Xiang, Wang, Shanyu, Hubble, Dion, Jang, Sei-Hum, Mueller, Karl T., Wang, Chongmin, Jen, Alex K.-Y., & Yang, Jihui. A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries. United States. https://doi.org/10.1039/c9ta02743b
Li, Yun, Murphy, Ian A., Chen, Ying, Li, Francis, Wang, Xiang, Wang, Shanyu, Hubble, Dion, Jang, Sei-Hum, Mueller, Karl T., Wang, Chongmin, Jen, Alex K.-Y., and Yang, Jihui. Wed . "A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries". United States. https://doi.org/10.1039/c9ta02743b.
@article{osti_1544787,
title = {A multi-functional interface derived from thiol-modified mesoporous carbon in lithium–sulfur batteries},
author = {Li, Yun and Murphy, Ian A. and Chen, Ying and Li, Francis and Wang, Xiang and Wang, Shanyu and Hubble, Dion and Jang, Sei-Hum and Mueller, Karl T. and Wang, Chongmin and Jen, Alex K.-Y. and Yang, Jihui},
abstractNote = {Lithium–sulfur (Li–S) batteries hold great promise as a next-generation energy-storage technology. Their practical application, however, is hindered by the rapid capacity fading associated with the dissolution of lithium polysulfides (LiPSs) into organic electrolytes. In this work, we successfully impede these losses by anchoring thiol (–SH) functional groups to the nonpolar surface of a mesoporous carbon host. This new strategy increases the surface polarity of conductive carbons and traps LiPSs inside cathodes. By utilizing various spectroscopic methods, we investigate the mechanisms of LiPS trapping, which originate from the electrostatic and covalent interactions of the thiol functional groups with Li+ from the electrolyte and with S from the LiPS chains, respectively. Here, we for the first time identify the multiple interactions that are induced by a small molecular interface upon cycling and correlate them with the electrochemical behavior. The fundamental insight on the thiol functionality suggests a further rational design of multifunctional interfaces to achieve better Li–S performance.},
doi = {10.1039/c9ta02743b},
url = {https://www.osti.gov/biblio/1544787}, journal = {Journal of Materials Chemistry A},
number = 21,
volume = 7,
place = {United States},
year = {2019},
month = {5}
}

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