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

Abstract

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.

Authors:
 [1];  [2];  [1];  [2];  [2];  [3];  [1]
+ Show Author Affiliations
  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:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
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); National Key Research and Development Program of China; National Natural Science Fund for Distinguished Young Scholars (China)
OSTI Identifier:
1417600
Alternate Identifier(s):
OSTI ID: 1396405
Grant/Contract Number:  
AC02-05CH11231; 2016YFA0202603; 51425204
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 38; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; nucleophilic substitution; poly(vinyl sulfate); carrageenan; chemical binding; high loading electrodes; lithium sulfur battery

Citation Formats

Ling, Min, Zhang, Liang, Zheng, Tianyue, Feng, Jun, Guo, Jinghua, Mai, Liqiang, and Liu, Gao. Nucleophilic substitution between polysulfides and binders unexpectedly stabilizing lithium sulfur battery. United States: N. p., 2017. Web. doi:10.1016/j.nanoen.2017.05.020.
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Ling, Min, Zhang, Liang, Zheng, Tianyue, Feng, Jun, Guo, Jinghua, Mai, Liqiang, & Liu, Gao. Nucleophilic substitution between polysulfides and binders unexpectedly stabilizing lithium sulfur battery. United States. https://doi.org/10.1016/j.nanoen.2017.05.020
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Ling, Min, Zhang, Liang, Zheng, Tianyue, Feng, Jun, Guo, Jinghua, Mai, Liqiang, and Liu, Gao. Wed . "Nucleophilic substitution between polysulfides and binders unexpectedly stabilizing lithium sulfur battery". United States. https://doi.org/10.1016/j.nanoen.2017.05.020. https://www.osti.gov/servlets/purl/1417600.
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@article{osti_1417600,
title = {Nucleophilic substitution between polysulfides and binders unexpectedly stabilizing lithium sulfur battery},
author = {Ling, Min and Zhang, Liang and Zheng, Tianyue and Feng, Jun and Guo, Jinghua and Mai, Liqiang and Liu, Gao},
abstractNote = {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/cm2, corresponding to 1199.1 mAh/g based on a micron-sulfur mass loading of 17.0 mg/cm2. 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/cm2, 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.},
doi = {10.1016/j.nanoen.2017.05.020},
url = {https://www.osti.gov/biblio/1417600}, journal = {Nano Energy},
issn = {2211-2855},
number = ,
volume = 38,
place = {United States},
year = {2017},
month = {5}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1016/j.nanoen.2017.05.020
Copyright Statement
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Works referencing / citing this record:

Understanding the Reaction Mechanism of Lithium–Sulfur Batteries by In Situ/Operando X-ray Absorption Spectroscopy
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Structural Design of Lithium–Sulfur Batteries: From Fundamental Research to Practical Application
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A Bifunctional Perovskite Promoter for Polysulfide Regulation toward Stable Lithium-Sulfur Batteries
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Understanding the Reaction Mechanism of Lithium–Sulfur Batteries by In Situ/Operando X-ray Absorption Spectroscopy
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Structural Design of Lithium–Sulfur Batteries: From Fundamental Research to Practical Application
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Sustainable Battery Materials from Biomass
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Porous Organic Polymers for Polysulfide Trapping in Lithium-Sulfur Batteries
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Current Status and Future Prospects of Metal–Sulfur Batteries
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A Review of Functional Binders in Lithium-Sulfur Batteries
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In Situ Techniques for Developing Robust Li-S Batteries
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Housing Sulfur in Polymer Composite Frameworks for Li–S Batteries
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Cathode porosity is a missing key parameter to optimize lithium-sulfur battery energy density
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Recent research trends in Li–S batteries
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Conductive molybdenum carbide as the polysulfide reservoir for lithium–sulfur batteries
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Vapour induced phase inversion: preparing high performance self-standing sponge-like electrodes with a sulfur loading of over 10 mg cm −2
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A robust and ion-conductive protein-based binder enabling strong polysulfide anchoring for high-energy lithium–sulfur batteries
journal, January 2019

In situ optical spectroscopy characterization for optimal design of lithium–sulfur batteries
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Inhibition of polysulfide diffusion in lithium–sulfur batteries: mechanism and improvement strategies
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Recent advances in polysulfide mediation of lithium-sulfur batteries via facile cathode and electrolyte modification
journal, August 2019

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