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Title: High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes

Abstract

This study examines the effects of nanophase S and surface coatings via atomic layer deposition (ALD) on high-loading sulfur cathodes for developing high-performance and high-energy lithium-sulfur (Li-S) batteries. It is first verified that ball milling is an effective and facile route for nanoengineering microsized S powders and the resultant nanoscale S particles exhibit better performance. Using these ball milled nanoscale S cathodes, it is found that ALD Al2O3 performed at 50 degrees C yields deposits that evolve with ALD cycles from dispersed nanoparticles, to porous, connected films, and finally to dense and continuous films. Moreover, this low temperature ALD process suppresses S loss by sublimation. The ALD Al2O3 greatly improves sulfur cathode sustainable capacity and Coulombic efficiency. This study postulates two different mechanisms underlying the effects of ALD Al2O3 surface coatings depending on their morphology. ALD Al2O3 nanoparticles dispersed on the sulfur surface mainly function to adsorb polysulfides, thereby inhibiting S shuttling and improving sustainable capacity and Coulombic efficiency. By contrast, ALD Al2O3 films behave as a physical barrier to prevent polysulfides from contacting the liquid electrolyte and dissolving. The dispersed Al2O3 nanoparticles improve both sustainable capacity and Coulombic efficiency while the closed Al2O3 films improve Coulombic efficiency while decreasingmore » the capacity« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [3]
+ Show Author Affiliations
  1. Department of Mechanical Engineering, University of Arkansas, Fayetteville AR 72701 USA
  2. Center for Nanoscale Materials, Argonne National Laboratory, Argonne IL 60439 USA
  3. Energy Systems Division, Argonne National Laboratory, Argonne IL 60439 USA
  4. Advanced Photon Source, Argonne National Laboratory, Argonne IL 60439 USA
  5. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne IL 60439 USA
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Joint Center for Energy Storage Research (JCESR)
OSTI Identifier:
1411012
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Advanced Materials Interfaces; Journal Volume: 4; Journal Issue: 17
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Li-sulfur batteries; atomic layer deposition; sulfur shuttling; surface coating

Citation Formats

Meng, Xiangbo, Liu, Yuzi, Cao, Yanqiang, Ren, Yang, Lu, Wenquan, and Elam, Jeffrey W. High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes. United States: N. p., 2017. Web. doi:10.1002/admi.201700096.
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Meng, Xiangbo, Liu, Yuzi, Cao, Yanqiang, Ren, Yang, Lu, Wenquan, & Elam, Jeffrey W. High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes. United States. doi:10.1002/admi.201700096.
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Meng, Xiangbo, Liu, Yuzi, Cao, Yanqiang, Ren, Yang, Lu, Wenquan, and Elam, Jeffrey W. Thu . "High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes". United States. doi:10.1002/admi.201700096.
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@article{osti_1411012,
title = {High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes},
author = {Meng, Xiangbo and Liu, Yuzi and Cao, Yanqiang and Ren, Yang and Lu, Wenquan and Elam, Jeffrey W.},
abstractNote = {This study examines the effects of nanophase S and surface coatings via atomic layer deposition (ALD) on high-loading sulfur cathodes for developing high-performance and high-energy lithium-sulfur (Li-S) batteries. It is first verified that ball milling is an effective and facile route for nanoengineering microsized S powders and the resultant nanoscale S particles exhibit better performance. Using these ball milled nanoscale S cathodes, it is found that ALD Al2O3 performed at 50 degrees C yields deposits that evolve with ALD cycles from dispersed nanoparticles, to porous, connected films, and finally to dense and continuous films. Moreover, this low temperature ALD process suppresses S loss by sublimation. The ALD Al2O3 greatly improves sulfur cathode sustainable capacity and Coulombic efficiency. This study postulates two different mechanisms underlying the effects of ALD Al2O3 surface coatings depending on their morphology. ALD Al2O3 nanoparticles dispersed on the sulfur surface mainly function to adsorb polysulfides, thereby inhibiting S shuttling and improving sustainable capacity and Coulombic efficiency. By contrast, ALD Al2O3 films behave as a physical barrier to prevent polysulfides from contacting the liquid electrolyte and dissolving. The dispersed Al2O3 nanoparticles improve both sustainable capacity and Coulombic efficiency while the closed Al2O3 films improve Coulombic efficiency while decreasing the capacity},
doi = {10.1002/admi.201700096},
journal = {Advanced Materials Interfaces},
number = 17,
volume = 4,
place = {United States},
year = {Thu May 18 00:00:00 EDT 2017},
month = {Thu May 18 00:00:00 EDT 2017}
}
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Journal Article:
DOI:  10.1002/admi.201700096
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  • ; ; ; ... - Advanced Materials Interfaces
    Cited by 1

  • ; ; ; ... - Scientific Reports
    The energy density of current lithium-ion batteries (LIBs) based on layered LiMO 2 cathodes (M=Ni, Mn, Co: NMC; M=Ni, Co, Al: NCA) needs to be improved significantly in order to compete with internal combustion engines and allow for widespread implementation of electric vehicles (EVs). In this report, we show that atomic layer deposition (ALD) of titania (TiO 2) and alumina (Al 2O 3) on Ni-rich FCG NMC and NCA active material particles could substantially improve LIB performance and allow for increased upper cutoff voltage (UCV) during charging, which delivers significantly increased specific energy utilization. Our results show that Al2O3 coatingmore » improved the NMC cycling performance by 40% and the NCA cycling performance by 34% at 1C/₋1C with respectively 4.35V and 4.4V UCV in 2Ah pouch cells. High resolution TEM/SAED structural characterization revealed that Al 2O 3 coatings prevented surface-initiated layered-to-spinel phase transitions in coated materials which were prevalent in uncoated materials. Lastly, EIS confirmed that Al 2O 3-coated materials had significantly lower increase in the charge transfer component of impedance during cycling. In conclusion, the ability to mitigate degradation mechanisms for Ni-rich NMC and NCA illustrated in this report provides insight into a method to enable the performance of high-voltage LIBs.« less
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  • ; ; ; ... - ACS Applied Materials and Interfaces

  • ; - ACS Energy Letters
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  • ; ; ; ... - Journal of Materials Chemistry A, 6(15):6617-6624
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