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Title: Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth

Abstract

Sulfur encapsulation in high surface area, nanoporous carbon is currently the most widely studied approach to improve the cycling stability of Li-S batteries. However, the relatively large amount of high surface area carbon decreases the overall volumetric energy density in the system and makes it difficult to compete with other battery chemistries. In this paper, we report a new approach that does not depend on sulfur encapsulation and high surface area carbon. We investigate the nucleation and deposition of sulfur using low surface area carbon in the cathode (surface area 17 m2 g-1). Optimization of the solvent properties and the deposition condition produce large spherical porous agglomerated particles rather than thin films. A solution mediated nucleation and growth mechanism is identified to form the large porous polysulfide particles. This new mechanism leads to close to 100% sulfur utilization, almost no capacity fading, over 99% coulombic efficacy, and high energy density (2350 Wh kg-1 and 2600 Wh L-1 based on overall mass/volume of cathode). This study may open a fundamentally new approach of using a low surface area carbon host for designing high energy Li-S battery by controlling the nucleation/growth pathway and morphology of sulfur species.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1406738
Report Number(s):
PNNL-SA-123317
Journal ID: ISSN 2058-7546; 48877; KC0208010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 2; Journal Issue: 10; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Pan, Huilin, Chen, Junzheng, Cao, Ruiguo, Murugesan, Vijay, Rajput, Nav Nidhi, Han, Kee Sung, Persson, Kristin, Estevez, Luis, Engelhard, Mark H., Zhang, Ji-Guang, Mueller, Karl T., Cui, Yi, Shao, Yuyan, and Liu, Jun. Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth. United States: N. p., 2017. Web. doi:10.1038/s41560-017-0005-z.
Pan, Huilin, Chen, Junzheng, Cao, Ruiguo, Murugesan, Vijay, Rajput, Nav Nidhi, Han, Kee Sung, Persson, Kristin, Estevez, Luis, Engelhard, Mark H., Zhang, Ji-Guang, Mueller, Karl T., Cui, Yi, Shao, Yuyan, & Liu, Jun. Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth. United States. doi:10.1038/s41560-017-0005-z.
Pan, Huilin, Chen, Junzheng, Cao, Ruiguo, Murugesan, Vijay, Rajput, Nav Nidhi, Han, Kee Sung, Persson, Kristin, Estevez, Luis, Engelhard, Mark H., Zhang, Ji-Guang, Mueller, Karl T., Cui, Yi, Shao, Yuyan, and Liu, Jun. Mon . "Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth". United States. doi:10.1038/s41560-017-0005-z.
@article{osti_1406738,
title = {Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth},
author = {Pan, Huilin and Chen, Junzheng and Cao, Ruiguo and Murugesan, Vijay and Rajput, Nav Nidhi and Han, Kee Sung and Persson, Kristin and Estevez, Luis and Engelhard, Mark H. and Zhang, Ji-Guang and Mueller, Karl T. and Cui, Yi and Shao, Yuyan and Liu, Jun},
abstractNote = {Sulfur encapsulation in high surface area, nanoporous carbon is currently the most widely studied approach to improve the cycling stability of Li-S batteries. However, the relatively large amount of high surface area carbon decreases the overall volumetric energy density in the system and makes it difficult to compete with other battery chemistries. In this paper, we report a new approach that does not depend on sulfur encapsulation and high surface area carbon. We investigate the nucleation and deposition of sulfur using low surface area carbon in the cathode (surface area 17 m2 g-1). Optimization of the solvent properties and the deposition condition produce large spherical porous agglomerated particles rather than thin films. A solution mediated nucleation and growth mechanism is identified to form the large porous polysulfide particles. This new mechanism leads to close to 100% sulfur utilization, almost no capacity fading, over 99% coulombic efficacy, and high energy density (2350 Wh kg-1 and 2600 Wh L-1 based on overall mass/volume of cathode). This study may open a fundamentally new approach of using a low surface area carbon host for designing high energy Li-S battery by controlling the nucleation/growth pathway and morphology of sulfur species.},
doi = {10.1038/s41560-017-0005-z},
journal = {Nature Energy},
issn = {2058-7546},
number = 10,
volume = 2,
place = {United States},
year = {2017},
month = {9}
}

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