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Title: Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries

Abstract

Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium-sulfur (Li-S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li-S pouch cells. In this work, we demonstrate that a rational combination of selenium doping, core-shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm-2) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm-2) with a low electrolyte/sulfur ratio (10 mu L mg(-1)). Overall, this research further demonstrates a durable Li-Se/S pouch cell with high specific capacity, validating the potential practical applications.

Authors:
 [1];  [2];  [3]; ORCiD logo [4]
  1. Hong Kong Univ. of Science and Technology, Kowloon (Hong Kong); Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Hong Kong Univ. of Science and Technology, Kowloon (Hong Kong)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); Stanford Univ., CA (United States); Imam Abdulrahman Bin Faisal Univ. (IAU), Dammam (Saudi Arabia)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Research Grants Council (RGC) of Hong Kong; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Vehicle Technologies (VTO), Battery Materials Research (BMR) Program; USDOE
OSTI Identifier:
1710199
Alternate Identifier(s):
OSTI ID: 1647286
Grant/Contract Number:  
AC02-06CH11357; T23-601/17-R; 16209218
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 40; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Cathode; High-energy-density batteries; Lithium metal anode; Selenium-sulfur; Solid-electrolyte interphase

Citation Formats

Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, and Amine, Khalil. Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries. United States: N. p., 2020. Web. https://doi.org/10.1002/anie.202007159.
Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, & Amine, Khalil. Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries. United States. https://doi.org/10.1002/anie.202007159
Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, and Amine, Khalil. Wed . "Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries". United States. https://doi.org/10.1002/anie.202007159. https://www.osti.gov/servlets/purl/1710199.
@article{osti_1710199,
title = {Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High-Energy Li-S Batteries},
author = {Zhao, Chen and Xu, Gui‐Liang and Zhao, Tianshou and Amine, Khalil},
abstractNote = {Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium-sulfur (Li-S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li-S pouch cells. In this work, we demonstrate that a rational combination of selenium doping, core-shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm-2) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm-2) with a low electrolyte/sulfur ratio (10 mu L mg(-1)). Overall, this research further demonstrates a durable Li-Se/S pouch cell with high specific capacity, validating the potential practical applications.},
doi = {10.1002/anie.202007159},
journal = {Angewandte Chemie (International Edition)},
number = 40,
volume = 59,
place = {United States},
year = {2020},
month = {8}
}

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